RADIONUCLIDE UPTAKE AND TRANSFER IN PELAGIC FOOD CHAINS OF THE BARENTS SEA AND RESULTING DOSES TO MAN AND

BIOTA

A project funded by the Norwegian Transport and Effects Programme, supported by the Norwegian Department of Foreign Affairs and Norwegian Department of the Environment

PREFACE

This project was a collaboration between the Norwegian Radiation Protection Authority (NRPA), the Institute of Marine Research, the Agricultural University of Norway, the Institute for Energy Technology and SPA TYPHOON, Russia. The work was funded by the Ministry of Foreign Affairs and the Ministry of Environment and co-ordinated through the Norwegian Polar Institute in collaboration with the NRPA.

CONTENT
1. Introduction 1 1.1 Present and potential sources of radionuclides 1 1.1.1 Global fallout 1 1.1.2 The Chernobyl accident 2 1.1.3 Western European Reprocessing plants 3 1.1.4 Other actual and potential sources of radioactivity to the northern marine environment 4 1.2 Prevailing regional marine currents 5 1.3 Mobility and biological uptake of radionuclides 7 1.3.1 Mobility 7 1.3.2 Biological uptake 9 1.4 Traditional impact assessments 10 1.5 Project objectives 12 1. Introduction...................................................................................................................19 1.1 Present and potential sources of radionuclides...............................................................19 1.1.1 Global fallout...........................................................................................................20 1.1.2 The Chernobyl accident...........................................................................................20 1.1.3 Western European Reprocessing plants...................................................................21 1.1.4 Other actual and potential sources of radioactivity to the northern marine environment......................................................................................................................22 1.2 Prevailing regional marine currents................................................................................23 1.3 Mobility and biological uptake of radionuclides............................................................25 1.3.1 Mobility....................................................................................................................25 1.3.2 Biological uptake.....................................................................................................27 1.4 Traditional impact assessments.......................................................................................28 1.5 Project objectives............................................................................................................30 2. Methodology..................................................................................................................34 2.1 Field work Barents Sea expedition January-February 1999........................................34 2.2 Sampling and pre-treatment of samples Barents Sea expedition January-February 1999 ...............................................................................................................................................35 2.2.1 Sampling of biota and sediment..............................................................................35 2.2.2 Pretreatment of sea water during field-work............................................................35 2.2.3 Ultrafiltration of Pu isotopes....................................................................................35 2.3 Laboratory studies...........................................................................................................35 2.4 Analyses of field samples from Barents Sea 1999 expedition........................................36 2.4.1 -emitting radionuclides..........................................................................................36 2.4.2 -emitting radionuclides..........................................................................................36 2.4.3 -emitting radionuclides..........................................................................................36 2.5 Human and biota dosimetric models...............................................................................37 3. Radionuclide activity concentrations in the environment..............................................38 3.1 Collation of data .............................................................................................................38 3.2 Results from the Barents Sea expedition 1999...............................................................40 3.2.1 Radionuclides in seawater........................................................................................40 3.2.2 Radionuclides in sediment.......................................................................................47 3.2.3 Radionuclides in biota..............................................................................................49 3.3 Caesium-137 and technetium-99 in seaweed..................................................................50 3.3.1 Materials and methods.............................................................................................51

3.3.2 Results and discussion.............................................................................................51 4. Mobility and uptake of radionuclides in marine systems..............................................57 4.1 Introduction.....................................................................................................................57 4.1.1 Mobility and bioavailability of radionuclides..........................................................57 4.2 Materials and methods....................................................................................................58 4.2.1 Mobility of radionuclides.........................................................................................58 4.2.2 Biotest experiments with Mytilus edulis .................................................................60 Sediment collection and characterisation..........................................................................60 Organism collection and handling....................................................................................60 Uptake experiments from tracers in ultrafiltered seawater...............................................60 Uptake experiments of tracers associated with suspended sediments..............................61 Depuration experiments....................................................................................................61 Tracer measurements........................................................................................................62 4.3 Results and discussion....................................................................................................63 4.3.1 Mobility of radionuclides - Results from Barents Sea field data.............................63 4.3.2 Bioavailability of radionuclides...............................................................................66 Activity levels in biota bioconcentration factors...........................................................66 Laboratory experiments - Uptake and depuration from ultrafiltered seawater................67 Table 4.4: Laboratory derived rate constants (Fig. 4.5) and BCFs for mussel soft parts (dry weight) when exposed to cationic tracers added to ultrafiltered seawater (Brretzen, 2001). ...............................................................................................................................................67 Ingestion and depuration of metals associated with particles...........................................69 4.4 Conclusions.....................................................................................................................70 5. Radionuclide uptake and transfer in pelagic food chains of the Barents Sea................72 5.1 Introduction.....................................................................................................................72 5.2 Materials and methods....................................................................................................74 5.3 Results and discussion....................................................................................................75 Specie................................................................................................................................77 5.4 Conclusion......................................................................................................................78 References..........................................................................................................................78 6. Ecological dosimetry models........................................................................................79 6.1 TYPHOON methodology...............................................................................................79 Under natural conditions, organisms are exposed to various sources of ionizing radiation. Absorbed dose to hydrobionts depends on a number of factors. Among them are type and energy of emitters (photons, beta particles, alpha particles, protons, neutrons, etc.), radiation source geometry (point or extended), space distribution and time evolution of radionuclide concentrations in components of aquatic ecosystems, ecologicalphysiological parameters and stage of ontogenesis of the organism (IAEA, 1976, 1979; Kryshev & Sazykina, 1986, 1990, 1995; Amiro, 1997; Sazykina et al., 1998). In the general case, the assessment of doses to organisms is an intricate problem. For the sake of simplicity, the dose rate assessments, as a rule, will be presented below for uniform distribution of radionuclides throughout the volume of organisms (for incorporated emitters) or environment (in calculations of external exposure)......................................79 6.1.1 Radiation dose from incorporated radionuclides.....................................................79 6.1.2 Radiation doses from external sources ....................................................................84 The dose rates to aquatic organisms from alpha and beta emitters scattered in the water depth are calculated with the following formulas:............................................................84 In many cases, when exposure to aquatic organisms nearby the surface of bottom sediments is considered, the sediments can be represented as an infinitely thick source with a uniformly distributed activity. In these cases, the beta- and gamma-radiation dose

rates nearby the surface of bottom sediments are equal to 0.5 P and 0.5 P, respectively. In the general case, as radionuclides are non-uniformly distributed in bottom sediments, the external gamma-radiation dose rate from the sediments to the organisms can be calculated with the formulas similar to Equation 6.16.........................84 6.1.3 Formalised algorithms..............................................................................................85 6.2 NRPA methodology.......................................................................................................85 6.3 Biota doses derived from archived data .........................................................................87 6.3.1 TYPHOON study....................................................................................................87 6.3.2 NRPA study.............................................................................................................87 6.3.3 Combined results .....................................................................................................89 6.4 Biota doses derived from the Barents Sea expedition 1999 - NRPA..............................89 6.4.1 Input data..................................................................................................................89 6.5 Biota doses derived from release scenarios TYPHOON.............................................90 6.5.1 Release scenario.......................................................................................................90 6.5.2 Results : Potential doses to marine biota in the Tsivolki Fjord (Realisation of the IASAP Scenario) ..............................................................................................................90 6.6 Interpretation of results in terms of dose-effects relationships.......................................91 7. Dose assessment for human populations .....................................................................94 7.1 TYPHOON methodology...............................................................................................94 7.2 NRPA methodology........................................................................................................95 One of the general assumptions for box modelling of the dispersion of radionuclides in marine system relates to instantaneous mixing in each box which, in term, results in practical calculations to an instantaneous mixing in the whole of oceanic space. A new approach for box modelling, which includes dispersion of radionuclides during time, was therefore created in order to provide a better and more realistic/physical approach comparing to traditional box modelling. Calculations of concentrations of radionuclides in the marine environment and doses for man for some scenarios indicate differences of up to orders of magnitude between the traditional and new approach for box modelling.............95 7.3 Human doses derived from archived data.......................................................................96 7.3.1 Individual doses.......................................................................................................96 7.3.2 Collective doses.......................................................................................................97 7.4 Human doses derived from release scenarios TYPHOON..........................................97 7.4.1 Assessment of the long-term radiological consequences of RW dumping in the Arctic Seas - TYPHOON..................................................................................................97 7.4.2 Assessment of the long-term radiological consequences for various discharge scenarios - NRPA..............................................................................................................98 8. Development of guidelines for vulnerability assessment............................................100 8.1 Introduction...................................................................................................................100 8.2 Considerations for a radioecological sensitivity assessment .......................................100 8.2.1 Abiotic....................................................................................................................101 8.2.2 Biotic......................................................................................................................103 8.3 What can be practically included in a radioecological sensitivity assessment ?...........104 8.3.1 A scenario for the quantification of Radioecological Sensitivity..........................105 8.4 Calculation of Radioecological sensitivity....................................................................106 8.5 Recent developments made, with respect to radiecological sensitivity analysis, within the Effects Programme....................................................................................................107 8.6 Recommendations for future monitoring programmes................................................109 8.6.1 Monitoring areas....................................................................................................109 8.6.2 Sampling programmes...........................................................................................110 1. Introduction...................................................................................................................19

1.1 Present and potential sources of radionuclides...............................................................19 1.1.1 Global fallout...........................................................................................................20 1.1.2 The Chernobyl accident...........................................................................................20 1.1.3 Western European Reprocessing plants...................................................................21 1.1.4 Other actual and potential sources of radioactivity to the northern marine environment......................................................................................................................22 1.2 Prevailing regional marine currents................................................................................23 1.3 Mobility and biological uptake of radionuclides............................................................25 1.3.1 Mobility....................................................................................................................25 1.3.2 Biological uptake.....................................................................................................27 1.4 Traditional impact assessments.......................................................................................28 1.5 Project objectives............................................................................................................30 2. Methodology..................................................................................................................34 2.1 Field work Barents Sea expedition January-February 1999........................................34 2.2 Sampling and pre-treatment of samples Barents Sea expedition January-February 1999 ...............................................................................................................................................35 2.2.1 Sampling of biota and sediment..............................................................................35 2.2.2 Pretreatment of sea water during field-work............................................................35 2.2.3 Ultrafiltration of Pu isotopes....................................................................................35 2.3 Laboratory studies...........................................................................................................35 2.4 Analyses of field samples from Barents Sea 1999 expedition........................................36 2.4.1 -emitting radionuclides..........................................................................................36 2.4.2 -emitting radionuclides..........................................................................................36 2.4.3 -emitting radionuclides..........................................................................................36 2.5 Human and biota dosimetric models...............................................................................37 3. Radionuclide activity concentrations in the environment..............................................38 3.1 Collation of data .............................................................................................................38 3.2 Results from the Barents Sea expedition 1999...............................................................40 3.2.1 Radionuclides in seawater........................................................................................40 3.2.2 Radionuclides in sediment.......................................................................................47 3.2.3 Radionuclides in biota..............................................................................................49 3.3 Caesium-137 and technetium-99 in seaweed..................................................................50 3.3.1 Materials and methods.............................................................................................51 3.3.2 Results and discussion.............................................................................................51 4. Mobility and uptake of radionuclides in marine systems..............................................57 4.1 Introduction.....................................................................................................................57 4.1.1 Mobility and bioavailability of radionuclides..........................................................57 4.2 Materials and methods....................................................................................................58 4.2.1 Mobility of radionuclides.........................................................................................58 4.2.2 Biotest experiments with Mytilus edulis .................................................................60 Sediment collection and characterisation..........................................................................60 Organism collection and handling....................................................................................60 Uptake experiments from tracers in ultrafiltered seawater...............................................60 Uptake experiments of tracers associated with suspended sediments..............................61 Depuration experiments....................................................................................................61 Tracer measurements........................................................................................................62 4.3 Results and discussion....................................................................................................63 4.3.1 Mobility of radionuclides - Results from Barents Sea field data.............................63 4.3.2 Bioavailability of radionuclides...............................................................................66 Activity levels in biota bioconcentration factors...........................................................66

Laboratory experiments - Uptake and depuration from ultrafiltered seawater................67 Table 4.4: Laboratory derived rate constants (Fig. 4.5) and BCFs for mussel soft parts (dry weight) when exposed to cationic tracers added to ultrafiltered seawater (Brretzen, 2001). ...............................................................................................................................................67 Ingestion and depuration of metals associated with particles...........................................69 4.4 Conclusions.....................................................................................................................70 5. Radionuclide uptake and transfer in pelagic food chains of the Barents Sea................72 5.1 Introduction.....................................................................................................................72 5.2 Materials and methods....................................................................................................74 5.3 Results and discussion....................................................................................................75 Specie................................................................................................................................77 5.4 Conclusion......................................................................................................................78 References..........................................................................................................................78 6. Ecological dosimetry models........................................................................................79 6.1 TYPHOON methodology...............................................................................................79 Under natural conditions, organisms are exposed to various sources of ionizing radiation. Absorbed dose to hydrobionts depends on a number of factors. Among them are type and energy of emitters (photons, beta particles, alpha particles, protons, neutrons, etc.), radiation source geometry (point or extended), space distribution and time evolution of radionuclide concentrations in components of aquatic ecosystems, ecologicalphysiological parameters and stage of ontogenesis of the organism (IAEA, 1976, 1979; Kryshev & Sazykina, 1986, 1990, 1995; Amiro, 1997; Sazykina et al., 1998). In the general case, the assessment of doses to organisms is an intricate problem. For the sake of simplicity, the dose rate assessments, as a rule, will be presented below for uniform distribution of radionuclides throughout the volume of organisms (for incorporated emitters) or environment (in calculations of external exposure)......................................79 6.1.1 Radiation dose from incorporated radionuclides.....................................................79 6.1.2 Radiation doses from external sources ....................................................................84 The dose rates to aquatic organisms from alpha and beta emitters scattered in the water depth are calculated with the following formulas:............................................................84 In many cases, when exposure to aquatic organisms nearby the surface of bottom sediments is considered, the sediments can be represented as an infinitely thick source with a uniformly distributed activity. In these cases, the beta- and gamma-radiation dose rates nearby the surface of bottom sediments are equal to 0.5 P and 0.5 P, respectively. In the general case, as radionuclides are non-uniformly distributed in bottom sediments, the external gamma-radiation dose rate from the sediments to the organisms can be calculated with the formulas similar to Equation 6.16.........................84 6.1.3 Formalised algorithms..............................................................................................85 6.2 NRPA methodology.......................................................................................................85 6.3 Biota doses derived from archived data .........................................................................87 6.3.1 TYPHOON study....................................................................................................87 6.3.2 NRPA study.............................................................................................................87 6.3.3 Combined results .....................................................................................................89 6.4 Biota doses derived from the Barents Sea expedition 1999 - NRPA..............................89 6.4.1 Input data..................................................................................................................89 6.5 Biota doses derived from release scenarios TYPHOON.............................................90 6.5.1 Release scenario.......................................................................................................90 6.5.2 Results : Potential doses to marine biota in the Tsivolki Fjord (Realisation of the IASAP Scenario) ..............................................................................................................90 6.6 Interpretation of results in terms of dose-effects relationships.......................................91

7. Dose assessment for human populations .....................................................................94 7.1 TYPHOON methodology...............................................................................................94 7.2 NRPA methodology........................................................................................................95 One of the general assumptions for box modelling of the dispersion of radionuclides in marine system relates to instantaneous mixing in each box which, in term, results in practical calculations to an instantaneous mixing in the whole of oceanic space. A new approach for box modelling, which includes dispersion of radionuclides during time, was therefore created in order to provide a better and more realistic/physical approach comparing to traditional box modelling. Calculations of concentrations of radionuclides in the marine environment and doses for man for some scenarios indicate differences of up to orders of magnitude between the traditional and new approach for box modelling.............95 7.3 Human doses derived from archived data.......................................................................96 7.3.1 Individual doses.......................................................................................................96 7.3.2 Collective doses.......................................................................................................97 7.4 Human doses derived from release scenarios TYPHOON..........................................97 7.4.1 Assessment of the long-term radiological consequences of RW dumping in the Arctic Seas - TYPHOON..................................................................................................97 7.4.2 Assessment of the long-term radiological consequences for various discharge scenarios - NRPA..............................................................................................................98 8. Development of guidelines for vulnerability assessment............................................100 8.1 Introduction...................................................................................................................100 8.2 Considerations for a radioecological sensitivity assessment .......................................100 8.2.1 Abiotic....................................................................................................................101 8.2.2 Biotic......................................................................................................................103 8.3 What can be practically included in a radioecological sensitivity assessment ?...........104 8.3.1 A scenario for the quantification of Radioecological Sensitivity..........................105 8.4 Calculation of Radioecological sensitivity....................................................................106 8.5 Recent developments made, with respect to radiecological sensitivity analysis, within the Effects Programme....................................................................................................107 8.6 Recommendations for future monitoring programmes................................................109 8.6.1 Monitoring areas....................................................................................................109 8.6.2 Sampling programmes...........................................................................................110 1. Introduction...................................................................................................................19 1.1 Present and potential sources of radionuclides...............................................................19 1.1.1 Global fallout...........................................................................................................20 1.1.2 The Chernobyl accident...........................................................................................20 1.1.3 Western European Reprocessing plants...................................................................21 1.1.4 Other actual and potential sources of radioactivity to the northern marine environment......................................................................................................................22 1.2 Prevailing regional marine currents................................................................................23 1.3 Mobility and biological uptake of radionuclides............................................................25 1.3.1 Mobility....................................................................................................................25 1.3.2 Biological uptake.....................................................................................................27 1.4 Traditional impact assessments.......................................................................................28 1.5 Project objectives............................................................................................................30 2. Methodology..................................................................................................................34 2.1 Field work Barents Sea expedition January-February 1999........................................34 2.2 Sampling and pre-treatment of samples Barents Sea expedition January-February 1999 ...............................................................................................................................................35 2.2.1 Sampling of biota and sediment..............................................................................35

2.2.2 Pretreatment of sea water during field-work............................................................35 2.2.3 Ultrafiltration of Pu isotopes....................................................................................35 2.3 Laboratory studies...........................................................................................................35 2.4 Analyses of field samples from Barents Sea 1999 expedition........................................36 2.4.1 -emitting radionuclides..........................................................................................36 2.4.2 -emitting radionuclides..........................................................................................36 2.4.3 -emitting radionuclides..........................................................................................36 2.5 Human and biota dosimetric models...............................................................................37 3. Radionuclide activity concentrations in the environment..............................................38 3.1 Collation of data .............................................................................................................38 3.2 Results from the Barents Sea expedition 1999...............................................................40 3.2.1 Radionuclides in seawater........................................................................................40 3.2.2 Radionuclides in sediment.......................................................................................47 3.2.3 Radionuclides in biota..............................................................................................49 3.3 Caesium-137 and technetium-99 in seaweed..................................................................50 3.3.1 Materials and methods.............................................................................................51 3.3.2 Results and discussion.............................................................................................51 4. Mobility and uptake of radionuclides in marine systems..............................................57 4.1 Introduction.....................................................................................................................57 4.1.1 Mobility and bioavailability of radionuclides..........................................................57 4.2 Materials and methods....................................................................................................58 4.2.1 Mobility of radionuclides.........................................................................................58 4.2.2 Biotest experiments with Mytilus edulis .................................................................60 Sediment collection and characterisation..........................................................................60 Organism collection and handling....................................................................................60 Uptake experiments from tracers in ultrafiltered seawater...............................................60 Uptake experiments of tracers associated with suspended sediments..............................61 Depuration experiments....................................................................................................61 Tracer measurements........................................................................................................62 4.3 Results and discussion....................................................................................................63 4.3.1 Mobility of radionuclides - Results from Barents Sea field data.............................63 4.3.2 Bioavailability of radionuclides...............................................................................66 Activity levels in biota bioconcentration factors...........................................................66 Laboratory experiments - Uptake and depuration from ultrafiltered seawater................67 Table 4.4: Laboratory derived rate constants (Fig. 4.5) and BCFs for mussel soft parts (dry weight) when exposed to cationic tracers added to ultrafiltered seawater (Brretzen, 2001). ...............................................................................................................................................67 Ingestion and depuration of metals associated with particles...........................................69 4.4 Conclusions.....................................................................................................................70 5. Radionuclide uptake and transfer in pelagic food chains of the Barents Sea................72 5.1 Introduction.....................................................................................................................72 5.2 Materials and methods....................................................................................................74 5.3 Results and discussion....................................................................................................75 Specie................................................................................................................................77 5.4 Conclusion......................................................................................................................78 References..........................................................................................................................78 6. Ecological dosimetry models........................................................................................79 6.1 TYPHOON methodology...............................................................................................79 Under natural conditions, organisms are exposed to various sources of ionizing radiation. Absorbed dose to hydrobionts depends on a number of factors. Among them are type and

energy of emitters (photons, beta particles, alpha particles, protons, neutrons, etc.), radiation source geometry (point or extended), space distribution and time evolution of radionuclide concentrations in components of aquatic ecosystems, ecologicalphysiological parameters and stage of ontogenesis of the organism (IAEA, 1976, 1979; Kryshev & Sazykina, 1986, 1990, 1995; Amiro, 1997; Sazykina et al., 1998). In the general case, the assessment of doses to organisms is an intricate problem. For the sake of simplicity, the dose rate assessments, as a rule, will be presented below for uniform distribution of radionuclides throughout the volume of organisms (for incorporated emitters) or environment (in calculations of external exposure)......................................79 6.1.1 Radiation dose from incorporated radionuclides.....................................................79 6.1.2 Radiation doses from external sources ....................................................................84 The dose rates to aquatic organisms from alpha and beta emitters scattered in the water depth are calculated with the following formulas:............................................................84 In many cases, when exposure to aquatic organisms nearby the surface of bottom sediments is considered, the sediments can be represented as an infinitely thick source with a uniformly distributed activity. In these cases, the beta- and gamma-radiation dose rates nearby the surface of bottom sediments are equal to 0.5 P and 0.5 P, respectively. In the general case, as radionuclides are non-uniformly distributed in bottom sediments, the external gamma-radiation dose rate from the sediments to the organisms can be calculated with the formulas similar to Equation 6.16.........................84 6.1.3 Formalised algorithms..............................................................................................85 6.2 NRPA methodology.......................................................................................................85 6.3 Biota doses derived from archived data .........................................................................87 6.3.1 TYPHOON study....................................................................................................87 6.3.2 NRPA study.............................................................................................................87 6.3.3 Combined results .....................................................................................................89 6.4 Biota doses derived from the Barents Sea expedition 1999 - NRPA..............................89 6.4.1 Input data..................................................................................................................89 6.5 Biota doses derived from release scenarios TYPHOON.............................................90 6.5.1 Release scenario.......................................................................................................90 6.5.2 Results : Potential doses to marine biota in the Tsivolki Fjord (Realisation of the IASAP Scenario) ..............................................................................................................90 6.6 Interpretation of results in terms of dose-effects relationships.......................................91 7. Dose assessment for human populations .....................................................................94 7.1 TYPHOON methodology...............................................................................................94 7.2 NRPA methodology........................................................................................................95 One of the general assumptions for box modelling of the dispersion of radionuclides in marine system relates to instantaneous mixing in each box which, in term, results in practical calculations to an instantaneous mixing in the whole of oceanic space. A new approach for box modelling, which includes dispersion of radionuclides during time, was therefore created in order to provide a better and more realistic/physical approach comparing to traditional box modelling. Calculations of concentrations of radionuclides in the marine environment and doses for man for some scenarios indicate differences of up to orders of magnitude between the traditional and new approach for box modelling.............95 7.3 Human doses derived from archived data.......................................................................96 7.3.1 Individual doses.......................................................................................................96 7.3.2 Collective doses.......................................................................................................97 7.4 Human doses derived from release scenarios TYPHOON..........................................97 7.4.1 Assessment of the long-term radiological consequences of RW dumping in the Arctic Seas - TYPHOON..................................................................................................97

7.4.2 Assessment of the long-term radiological consequences for various discharge scenarios - NRPA..............................................................................................................98 8. Development of guidelines for vulnerability assessment............................................100 8.1 Introduction...................................................................................................................100 8.2 Considerations for a radioecological sensitivity assessment .......................................100 8.2.1 Abiotic....................................................................................................................101 8.2.2 Biotic......................................................................................................................103 8.3 What can be practically included in a radioecological sensitivity assessment ?...........104 8.3.1 A scenario for the quantification of Radioecological Sensitivity..........................105 8.4 Calculation of Radioecological sensitivity....................................................................106 8.5 Recent developments made, with respect to radiecological sensitivity analysis, within the Effects Programme....................................................................................................107 8.6 Recommendations for future monitoring programmes................................................109 8.6.1 Monitoring areas....................................................................................................109 8.6.2 Sampling programmes...........................................................................................110 1. Introduction...................................................................................................................19 1.1 Present and potential sources of radionuclides...............................................................19 1.1.1 Global fallout...........................................................................................................20 1.1.2 The Chernobyl accident...........................................................................................20 1.1.3 Western European Reprocessing plants...................................................................21 1.1.4 Other actual and potential sources of radioactivity to the northern marine environment......................................................................................................................22 1.2 Prevailing regional marine currents................................................................................23 1.3 Mobility and biological uptake of radionuclides............................................................25 1.3.1 Mobility....................................................................................................................25 1.3.2 Biological uptake.....................................................................................................27 1.4 Traditional impact assessments.......................................................................................28 1.5 Project objectives............................................................................................................30 2. Methodology..................................................................................................................34 2.1 Field work Barents Sea expedition January-February 1999........................................34 2.2 Sampling and pre-treatment of samples Barents Sea expedition January-February 1999 ...............................................................................................................................................35 2.2.1 Sampling of biota and sediment..............................................................................35 2.2.2 Pretreatment of sea water during field-work............................................................35 2.2.3 Ultrafiltration of Pu isotopes....................................................................................35 2.3 Laboratory studies...........................................................................................................35 2.4 Analyses of field samples from Barents Sea 1999 expedition........................................36 2.4.1 -emitting radionuclides..........................................................................................36 2.4.2 -emitting radionuclides..........................................................................................36 2.4.3 -emitting radionuclides..........................................................................................36 2.5 Human and biota dosimetric models...............................................................................37 3. Radionuclide activity concentrations in the environment..............................................38 3.1 Collation of data .............................................................................................................38 3.2 Results from the Barents Sea expedition 1999...............................................................40 3.2.1 Radionuclides in seawater........................................................................................40 3.2.2 Radionuclides in sediment.......................................................................................47 3.2.3 Radionuclides in biota..............................................................................................49 3.3 Caesium-137 and technetium-99 in seaweed..................................................................50 3.3.1 Materials and methods.............................................................................................51 3.3.2 Results and discussion.............................................................................................51

4. Mobility and uptake of radionuclides in marine systems..............................................57 4.1 Introduction.....................................................................................................................57 4.1.1 Mobility and bioavailability of radionuclides..........................................................57 4.2 Materials and methods....................................................................................................58 4.2.1 Mobility of radionuclides.........................................................................................58 4.2.2 Biotest experiments with Mytilus edulis .................................................................60 Sediment collection and characterisation..........................................................................60 Organism collection and handling....................................................................................60 Uptake experiments from tracers in ultrafiltered seawater...............................................60 Uptake experiments of tracers associated with suspended sediments..............................61 Depuration experiments....................................................................................................61 Tracer measurements........................................................................................................62 4.3 Results and discussion....................................................................................................63 4.3.1 Mobility of radionuclides - Results from Barents Sea field data.............................63 4.3.2 Bioavailability of radionuclides...............................................................................66 Activity levels in biota bioconcentration factors...........................................................66 Laboratory experiments - Uptake and depuration from ultrafiltered seawater................67 Table 4.4: Laboratory derived rate constants (Fig. 4.5) and BCFs for mussel soft parts (dry weight) when exposed to cationic tracers added to ultrafiltered seawater (Brretzen, 2001). ...............................................................................................................................................67 Ingestion and depuration of metals associated with particles...........................................69 4.4 Conclusions.....................................................................................................................70 5. Radionuclide uptake and transfer in pelagic food chains of the Barents Sea................72 5.1 Introduction.....................................................................................................................72 5.2 Materials and methods....................................................................................................74 5.3 Results and discussion....................................................................................................75 Specie................................................................................................................................77 5.4 Conclusion......................................................................................................................78 References..........................................................................................................................78 6. Ecological dosimetry models........................................................................................79 6.1 TYPHOON methodology...............................................................................................79 Under natural conditions, organisms are exposed to various sources of ionizing radiation. Absorbed dose to hydrobionts depends on a number of factors. Among them are type and energy of emitters (photons, beta particles, alpha particles, protons, neutrons, etc.), radiation source geometry (point or extended), space distribution and time evolution of radionuclide concentrations in components of aquatic ecosystems, ecologicalphysiological parameters and stage of ontogenesis of the organism (IAEA, 1976, 1979; Kryshev & Sazykina, 1986, 1990, 1995; Amiro, 1997; Sazykina et al., 1998). In the general case, the assessment of doses to organisms is an intricate problem. For the sake of simplicity, the dose rate assessments, as a rule, will be presented below for uniform distribution of radionuclides throughout the volume of organisms (for incorporated emitters) or environment (in calculations of external exposure)......................................79 6.1.1 Radiation dose from incorporated radionuclides.....................................................79 6.1.2 Radiation doses from external sources ....................................................................84 The dose rates to aquatic organisms from alpha and beta emitters scattered in the water depth are calculated with the following formulas:............................................................84 In many cases, when exposure to aquatic organisms nearby the surface of bottom sediments is considered, the sediments can be represented as an infinitely thick source with a uniformly distributed activity. In these cases, the beta- and gamma-radiation dose rates nearby the surface of bottom sediments are equal to 0.5 P and 0.5 P,

respectively. In the general case, as radionuclides are non-uniformly distributed in bottom sediments, the external gamma-radiation dose rate from the sediments to the organisms can be calculated with the formulas similar to Equation 6.16.........................84 6.1.3 Formalised algorithms..............................................................................................85 6.2 NRPA methodology.......................................................................................................85 6.3 Biota doses derived from archived data .........................................................................87 6.3.1 TYPHOON study....................................................................................................87 6.3.2 NRPA study.............................................................................................................87 6.3.3 Combined results .....................................................................................................89 6.4 Biota doses derived from the Barents Sea expedition 1999 - NRPA..............................89 6.4.1 Input data..................................................................................................................89 6.5 Biota doses derived from release scenarios TYPHOON.............................................90 6.5.1 Release scenario.......................................................................................................90 6.5.2 Results : Potential doses to marine biota in the Tsivolki Fjord (Realisation of the IASAP Scenario) ..............................................................................................................90 6.6 Interpretation of results in terms of dose-effects relationships.......................................91 7. Dose assessment for human populations .....................................................................94 7.1 TYPHOON methodology...............................................................................................94 7.2 NRPA methodology........................................................................................................95 One of the general assumptions for box modelling of the dispersion of radionuclides in marine system relates to instantaneous mixing in each box which, in term, results in practical calculations to an instantaneous mixing in the whole of oceanic space. A new approach for box modelling, which includes dispersion of radionuclides during time, was therefore created in order to provide a better and more realistic/physical approach comparing to traditional box modelling. Calculations of concentrations of radionuclides in the marine environment and doses for man for some scenarios indicate differences of up to orders of magnitude between the traditional and new approach for box modelling.............95 7.3 Human doses derived from archived data.......................................................................96 7.3.1 Individual doses.......................................................................................................96 7.3.2 Collective doses.......................................................................................................97 7.4 Human doses derived from release scenarios TYPHOON..........................................97 7.4.1 Assessment of the long-term radiological consequences of RW dumping in the Arctic Seas - TYPHOON..................................................................................................97 7.4.2 Assessment of the long-term radiological consequences for various discharge scenarios - NRPA..............................................................................................................98 8. Development of guidelines for vulnerability assessment............................................100 8.1 Introduction...................................................................................................................100 8.2 Considerations for a radioecological sensitivity assessment .......................................100 8.2.1 Abiotic....................................................................................................................101 8.2.2 Biotic......................................................................................................................103 8.3 What can be practically included in a radioecological sensitivity assessment ?...........104 8.3.1 A scenario for the quantification of Radioecological Sensitivity..........................105 8.4 Calculation of Radioecological sensitivity....................................................................106 8.5 Recent developments made, with respect to radiecological sensitivity analysis, within the Effects Programme....................................................................................................107 8.6 Recommendations for future monitoring programmes................................................109 8.6.1 Monitoring areas....................................................................................................109 8.6.2 Sampling programmes...........................................................................................110 1. Introduction...................................................................................................................19 1.1 Present and potential sources of radionuclides...............................................................19

1.1.1 Global fallout...........................................................................................................20 1.1.2 The Chernobyl accident...........................................................................................20 1.1.3 Western European Reprocessing plants...................................................................21 1.1.4 Other actual and potential sources of radioactivity to the northern marine environment......................................................................................................................22 1.2 Prevailing regional marine currents................................................................................23 1.3 Mobility and biological uptake of radionuclides............................................................25 1.3.1 Mobility....................................................................................................................25 1.3.2 Biological uptake.....................................................................................................27 1.4 Traditional impact assessments.......................................................................................28 1.5 Project objectives............................................................................................................30 2. Methodology..................................................................................................................34 2.1 Field work Barents Sea expedition January-February 1999........................................34 2.2 Sampling and pre-treatment of samples Barents Sea expedition January-February 1999 ...............................................................................................................................................35 2.2.1 Sampling of biota and sediment..............................................................................35 2.2.2 Pretreatment of sea water during field-work............................................................35 2.2.3 Ultrafiltration of Pu isotopes....................................................................................35 2.3 Laboratory studies...........................................................................................................35 2.4 Analyses of field samples from Barents Sea 1999 expedition........................................36 2.4.1 -emitting radionuclides..........................................................................................36 2.4.2 -emitting radionuclides..........................................................................................36 2.4.3 -emitting radionuclides..........................................................................................36 2.5 Human and biota dosimetric models...............................................................................37 3. Radionuclide activity concentrations in the environment..............................................38 3.1 Collation of data .............................................................................................................38 3.2 Results from the Barents Sea expedition 1999...............................................................40 3.2.1 Radionuclides in seawater........................................................................................40 3.2.2 Radionuclides in sediment.......................................................................................47 3.2.3 Radionuclides in biota..............................................................................................49 3.3 Caesium-137 and technetium-99 in seaweed..................................................................50 3.3.1 Materials and methods.............................................................................................51 3.3.2 Results and discussion.............................................................................................51 4. Mobility and uptake of radionuclides in marine systems..............................................57 4.1 Introduction.....................................................................................................................57 4.1.1 Mobility and bioavailability of radionuclides..........................................................57 4.2 Materials and methods....................................................................................................58 4.2.1 Mobility of radionuclides.........................................................................................58 4.2.2 Biotest experiments with Mytilus edulis .................................................................60 Sediment collection and characterisation..........................................................................60 Organism collection and handling....................................................................................60 Uptake experiments from tracers in ultrafiltered seawater...............................................60 Uptake experiments of tracers associated with suspended sediments..............................61 Depuration experiments....................................................................................................61 Tracer measurements........................................................................................................62 4.3 Results and discussion....................................................................................................63 4.3.1 Mobility of radionuclides - Results from Barents Sea field data.............................63 4.3.2 Bioavailability of radionuclides...............................................................................66 Activity levels in biota bioconcentration factors...........................................................66 Laboratory experiments - Uptake and depuration from ultrafiltered seawater................67

Table 4.4: Laboratory derived rate constants (Fig. 4.5) and BCFs for mussel soft parts (dry weight) when exposed to cationic tracers added to ultrafiltered seawater (Brretzen, 2001). ...............................................................................................................................................67 Ingestion and depuration of metals associated with particles...........................................69 4.4 Conclusions.....................................................................................................................70 5. Radionuclide uptake and transfer in pelagic food chains of the Barents Sea................72 5.1 Introduction.....................................................................................................................72 5.2 Materials and methods....................................................................................................74 5.3 Results and discussion....................................................................................................75 Specie................................................................................................................................77 5.4 Conclusion......................................................................................................................78 References..........................................................................................................................78 6. Ecological dosimetry models........................................................................................79 6.1 TYPHOON methodology...............................................................................................79 Under natural conditions, organisms are exposed to various sources of ionizing radiation. Absorbed dose to hydrobionts depends on a number of factors. Among them are type and energy of emitters (photons, beta particles, alpha particles, protons, neutrons, etc.), radiation source geometry (point or extended), space distribution and time evolution of radionuclide concentrations in components of aquatic ecosystems, ecologicalphysiological parameters and stage of ontogenesis of the organism (IAEA, 1976, 1979; Kryshev & Sazykina, 1986, 1990, 1995; Amiro, 1997; Sazykina et al., 1998). In the general case, the assessment of doses to organisms is an intricate problem. For the sake of simplicity, the dose rate assessments, as a rule, will be presented below for uniform distribution of radionuclides throughout the volume of organisms (for incorporated emitters) or environment (in calculations of external exposure)......................................79 6.1.1 Radiation dose from incorporated radionuclides.....................................................79 6.1.2 Radiation doses from external sources ....................................................................84 The dose rates to aquatic organisms from alpha and beta emitters scattered in the water depth are calculated with the following formulas:............................................................84 In many cases, when exposure to aquatic organisms nearby the surface of bottom sediments is considered, the sediments can be represented as an infinitely thick source with a uniformly distributed activity. In these cases, the beta- and gamma-radiation dose rates nearby the surface of bottom sediments are equal to 0.5 P and 0.5 P, respectively. In the general case, as radionuclides are non-uniformly distributed in bottom sediments, the external gamma-radiation dose rate from the sediments to the organisms can be calculated with the formulas similar to Equation 6.16.........................84 6.1.3 Formalised algorithms..............................................................................................85 6.2 NRPA methodology.......................................................................................................85 6.3 Biota doses derived from archived data .........................................................................87 6.3.1 TYPHOON study....................................................................................................87 6.3.2 NRPA study.............................................................................................................87 6.3.3 Combined results .....................................................................................................89 6.4 Biota doses derived from the Barents Sea expedition 1999 - NRPA..............................89 6.4.1 Input data..................................................................................................................89 6.5 Biota doses derived from release scenarios TYPHOON.............................................90 6.5.1 Release scenario.......................................................................................................90 6.5.2 Results : Potential doses to marine biota in the Tsivolki Fjord (Realisation of the IASAP Scenario) ..............................................................................................................90 6.6 Interpretation of results in terms of dose-effects relationships.......................................91 7. Dose assessment for human populations .....................................................................94

7.1 TYPHOON methodology...............................................................................................94 7.2 NRPA methodology........................................................................................................95 One of the general assumptions for box modelling of the dispersion of radionuclides in marine system relates to instantaneous mixing in each box which, in term, results in practical calculations to an instantaneous mixing in the whole of oceanic space. A new approach for box modelling, which includes dispersion of radionuclides during time, was therefore created in order to provide a better and more realistic/physical approach comparing to traditional box modelling. Calculations of concentrations of radionuclides in the marine environment and doses for man for some scenarios indicate differences of up to orders of magnitude between the traditional and new approach for box modelling.............95 7.3 Human doses derived from archived data.......................................................................96 7.3.1 Individual doses.......................................................................................................96 7.3.2 Collective doses.......................................................................................................97 7.4 Human doses derived from release scenarios TYPHOON..........................................97 7.4.1 Assessment of the long-term radiological consequences of RW dumping in the Arctic Seas - TYPHOON..................................................................................................97 7.4.2 Assessment of the long-term radiological consequences for various discharge scenarios - NRPA..............................................................................................................98 8. Development of guidelines for vulnerability assessment............................................100 8.1 Introduction...................................................................................................................100 8.2 Considerations for a radioecological sensitivity assessment .......................................100 8.2.1 Abiotic....................................................................................................................101 8.2.2 Biotic......................................................................................................................103 8.3 What can be practically included in a radioecological sensitivity assessment ?...........104 8.3.1 A scenario for the quantification of Radioecological Sensitivity..........................105 8.4 Calculation of Radioecological sensitivity....................................................................106 8.5 Recent developments made, with respect to radiecological sensitivity analysis, within the Effects Programme....................................................................................................107 8.6 Recommendations for future monitoring programmes................................................109 8.6.1 Monitoring areas....................................................................................................109 8.6.2 Sampling programmes...........................................................................................110 1. Introduction...................................................................................................................19 1.1 Present and potential sources of radionuclides...............................................................19 1.1.1 Global fallout...........................................................................................................20 1.1.2 The Chernobyl accident...........................................................................................20 1.1.3 Western European Reprocessing plants...................................................................21 1.1.4 Other actual and potential sources of radioactivity to the northern marine environment......................................................................................................................22 1.2 Prevailing regional marine currents................................................................................23 1.3 Mobility and biological uptake of radionuclides............................................................25 1.3.1 Mobility....................................................................................................................25 1.3.2 Biological uptake.....................................................................................................27 1.4 Traditional impact assessments.......................................................................................28 1.5 Project objectives............................................................................................................30 2. Methodology..................................................................................................................34 2.1 Field work Barents Sea expedition January-February 1999........................................34 2.2 Sampling and pre-treatment of samples Barents Sea expedition January-February 1999 ...............................................................................................................................................35 2.2.1 Sampling of biota and sediment..............................................................................35

2.2.2 Pretreatment of sea water during field-work............................................................35 2.2.3 Ultrafiltration of Pu isotopes....................................................................................35 2.3 Laboratory studies...........................................................................................................35 2.4 Analyses of field samples from Barents Sea 1999 expedition........................................36 2.4.1 -emitting radionuclides..........................................................................................36 2.4.2 -emitting radionuclides..........................................................................................36 2.4.3 -emitting radionuclides..........................................................................................36 2.5 Human and biota dosimetric models...............................................................................37 3. Radionuclide activity concentrations in the environment..............................................38 3.1 Collation of data .............................................................................................................38 3.2 Results from the Barents Sea expedition 1999...............................................................40 3.2.1 Radionuclides in seawater........................................................................................40 3.2.2 Radionuclides in sediment.......................................................................................47 3.2.3 Radionuclides in biota..............................................................................................49 3.3 Caesium-137 and technetium-99 in seaweed..................................................................50 3.3.1 Materials and methods.............................................................................................51 3.3.2 Results and discussion.............................................................................................51 4. Mobility and uptake of radionuclides in marine systems..............................................57 4.1 Introduction.....................................................................................................................57 4.1.1 Mobility and bioavailability of radionuclides..........................................................57 4.2 Materials and methods....................................................................................................58 4.2.1 Mobility of radionuclides.........................................................................................58 4.2.2 Biotest experiments with Mytilus edulis .................................................................60 Sediment collection and characterisation..........................................................................60 Organism collection and handling....................................................................................60 Uptake experiments from tracers in ultrafiltered seawater...............................................60 Uptake experiments of tracers associated with suspended sediments..............................61 Depuration experiments....................................................................................................61 Tracer measurements........................................................................................................62 4.3 Results and discussion....................................................................................................63 4.3.1 Mobility of radionuclides - Results from Barents Sea field data.............................63 4.3.2 Bioavailability of radionuclides...............................................................................66 Activity levels in biota bioconcentration factors...........................................................66 Laboratory experiments - Uptake and depuration from ultrafiltered seawater................67 Table 4.4: Laboratory derived rate constants (Fig. 4.5) and BCFs for mussel soft parts (dry weight) when exposed to cationic tracers added to ultrafiltered seawater (Brretzen, 2001). ...............................................................................................................................................67 Ingestion and depuration of metals associated with particles...........................................69 4.4 Conclusions.....................................................................................................................70 5. Radionuclide uptake and transfer in pelagic food chains of the Barents Sea................72 5.1 Introduction.....................................................................................................................72 5.2 Materials and methods....................................................................................................74 5.3 Results and discussion....................................................................................................75 Specie................................................................................................................................77 5.4 Conclusion......................................................................................................................78 References..........................................................................................................................78 6. Ecological dosimetry models........................................................................................79 6.1 TYPHOON methodology...............................................................................................79 Under natural conditions, organisms are exposed to various sources of ionizing radiation. Absorbed dose to hydrobionts depends on a number of factors. Among them are type and

energy of emitters (photons, beta particles, alpha particles, protons, neutrons, etc.), radiation source geometry (point or extended), space distribution and time evolution of radionuclide concentrations in components of aquatic ecosystems, ecologicalphysiological parameters and stage of ontogenesis of the organism (IAEA, 1976, 1979; Kryshev & Sazykina, 1986, 1990, 1995; Amiro, 1997; Sazykina et al., 1998). In the general case, the assessment of doses to organisms is an intricate problem. For the sake of simplicity, the dose rate assessments, as a rule, will be presented below for uniform distribution of radionuclides throughout the volume of organisms (for incorporated emitters) or environment (in calculations of external exposure)......................................79 6.1.1 Radiation dose from incorporated radionuclides.....................................................79 6.1.2 Radiation doses from external sources ....................................................................84 The dose rates to aquatic organisms from alpha and beta emitters scattered in the water depth are calculated with the following formulas:............................................................84 In many cases, when exposure to aquatic organisms nearby the surface of bottom sediments is considered, the sediments can be represented as an infinitely thick source with a uniformly distributed activity. In these cases, the beta- and gamma-radiation dose rates nearby the surface of bottom sediments are equal to 0.5 P and 0.5 P, respectively. In the general case, as radionuclides are non-uniformly distributed in bottom sediments, the external gamma-radiation dose rate from the sediments to the organisms can be calculated with the formulas similar to Equation 6.16.........................84 6.1.3 Formalised algorithms..............................................................................................85 6.2 NRPA methodology.......................................................................................................85 6.3 Biota doses derived from archived data .........................................................................87 6.3.1 TYPHOON study....................................................................................................87 6.3.2 NRPA study.............................................................................................................87 6.3.3 Combined results .....................................................................................................89 6.4 Biota doses derived from the Barents Sea expedition 1999 - NRPA..............................89 6.4.1 Input data..................................................................................................................89 6.5 Biota doses derived from release scenarios TYPHOON.............................................90 6.5.1 Release scenario.......................................................................................................90 6.5.2 Results : Potential doses to marine biota in the Tsivolki Fjord (Realisation of the IASAP Scenario) ..............................................................................................................90 6.6 Interpretation of results in terms of dose-effects relationships.......................................91 7. Dose assessment for human populations .....................................................................94 7.1 TYPHOON methodology...............................................................................................94 7.2 NRPA methodology........................................................................................................95 One of the general assumptions for box modelling of the dispersion of radionuclides in marine system relates to instantaneous mixing in each box which, in term, results in practical calculations to an instantaneous mixing in the whole of oceanic space. A new approach for box modelling, which includes dispersion of radionuclides during time, was therefore created in order to provide a better and more realistic/physical approach comparing to traditional box modelling. Calculations of concentrations of radionuclides in the marine environment and doses for man for some scenarios indicate differences of up to orders of magnitude between the traditional and new approach for box modelling.............95 7.3 Human doses derived from archived data.......................................................................96 7.3.1 Individual doses.......................................................................................................96 7.3.2 Collective doses.......................................................................................................97 7.4 Human doses derived from release scenarios TYPHOON..........................................97 7.4.1 Assessment of the long-term radiological consequences of RW dumping in the Arctic Seas - TYPHOON..................................................................................................97

7.4.2 Assessment of the long-term radiological consequences for various discharge scenarios - NRPA..............................................................................................................98 8. Development of guidelines for vulnerability assessment............................................100 8.1 Introduction...................................................................................................................100 8.2 Considerations for a radioecological sensitivity assessment .......................................100 8.2.1 Abiotic....................................................................................................................101 8.2.2 Biotic......................................................................................................................103 8.3 What can be practically included in a radioecological sensitivity assessment ?...........104 8.3.1 A scenario for the quantification of Radioecological Sensitivity..........................105 8.4 Calculation of Radioecological sensitivity....................................................................106 8.5 Recent developments made, with respect to radiecological sensitivity analysis, within the Effects Programme....................................................................................................107 8.6 Recommendations for future monitoring programmes................................................109 8.6.1 Monitoring areas....................................................................................................109 8.6.2 Sampling programmes...........................................................................................110

1. Introduction
Authors : Justin Brown & Siri Grttheim Norwegian Radiation Protection Authority This report summarises the work conducted within the project Radionuclide uptake and transfer in pelagic food chains of the Barents Sea and resulting doses to Man and biota. The report is split into 8 Chapters dealing with the various themes specified in the project description. Chapter 1 considers both actual and potential sources of radionuclides to the environment, how these contaminants are dispersed and transferred to living organisms. The traditional methods of radiological impact assessment along with proposed changes in the way such assessments might be conducted are also explored. The field expedition, sampling and analytical methodologies are presented in Chapter 2 and the results from the main fieldwork conducted within the framework of this project are presented in Chapter 3. The topic of Chapter 4 is mobility of radionuclides and uptake by organisms in the marine environment and forms the main input from the Agricultural University of Norway (AUN). Chapter 5 is entitled Radionuclide uptake and transfer in pelagic food chains of the Barents Sea and forms the main input from the Institute of Marine Research (IMR) and the Institute for Energy Technology (IFE). Chapters 6 & 7 deal with radiological dose assessments for man and biota and combine the work of SPA TYPHOON and the Norwegian Radiation Protection Authority (NRPA). The final chapter, written by the NRPA, considers guidelines for a vulnerability assessment in marine environments.

1.1 Present and potential sources of radionuclides

In addition to naturally-occurring radionuclides in water masses and sediments of the marine environment, a number of artificial radionuclides have been produced and released to sea water. The major contributions of artificial radionuclides to the northern marine environment, defined as an area which includes the Barents Sea and Norwegian Sea, originate from global fallout from previous atmospheric nuclear weapons tests, discharges from the Sellafield spent nuclear fuel reprocessing plant (UK) and fallout from the accident at the Chernobyl nuclear power plant (Ukraine) in 1986 .

1.1.1 Global fallout

In a global perspective, the dominating radioactive contamination source is global fallout of debris from the atmospheric nuclear bomb tests conducted in different parts of the world between 1945 and 1980. In total, 520 atmospheric nuclear explosions were carried out, with periods of most intensive testing in the years 1952-1954, 1957-1958 and 1961-1962 (UNSCEAR, 1993). Atmospheric nuclear weapons tests were mainly conducted by the United States, the Soviet Union, the United Kingdom, France and the Peoples Republic of China. The three major tests sites for atmospheric testing were Novaya Zemlya (Russia) in the Arctic Ocean, the Bikini and Eniwetok Islands (USA) in the Pacific Ocean and the Nevada test site (USA) (Strand et al., 1998). It has been concluded that 12% of the fallout activity has been deposited close to the test site, 10% has been deposited in a band around the earth at the latitude of the test site (tropospheric fallout) and 78% of the fallout activity has been spread over larger areas, and mostly in the same hemisphere as the test site, producing global fallout (UNSCEAR, 1993). As most of the weapons tests have been carried out in the northern hemisphere, the largest radioactive contamination is found there. These weapons tests have contributed to an overall background contamination level of long-lived fission products and transuranics in the northern marine environment. In terms of specific radionuclide releases, some 600 PBq 90Sr was released in the period 1952-1962 compared to a 910 PBq release of 137 Cs (Balonov, 1997).

1.1.2 The Chernobyl accident

In addition to atmospheric nuclear weapons test, the accident at the Chernobyl nuclear power plant in the Ukraine (see Figure 1.1) on April 26, 1986, was the second significant large-scale fallout source of environmental radioactive contamination to the Arctic (Strand et al., 1998). The accident was a consequence of uncontrolled fission in the reactor, followed by a powerful explosion and fire. The radioactive materials released were carried away in the form of gases and dust particles by air currents. They were widely dispersed over the Soviet Union and several European countries (UNSCEAR, 1988). Whereas the weapons tests produced almost no 134Cs, the 134Cs to 137Cs ratio, in fallout from Chernobyl, was approximately 1:2 (in April 1986) (IAEA, 1986). This ratio can be used to trace Chernobyl-derived radiocaesium Currently, regarding the northern seas, the main contribution to Chernobyl-derived radiocaesium originates from the heavily contaminated Baltic Sea, reaching the northern marine environment by ocean currents: According to Josefsson (1998), more than 90% of the net outflow of 137Cs from the Baltic consists of Chernobyl activity. Only 8 PBq of 90Sr compared to 85 PBq 137Cs was released during the Chernobyl accident on a regional scale (Strand et al., 1998). The total release of -emitting plutonium nuclides from the Chernobyl accident was approximately 0.1 PBq. Furthermore, most of the plutonium nuclides released from the accident were deposited in the vicinity of Chernobyl (Strand et al., 1998). This indicates that the accident has contributed with very low levels of plutonium to the marine environment.

Figure 1.1 : Sources of radionuclides to northern marine environments : Chernobyl in the Ukraine, the reprocessing plants at Sellafield, La Hague and Dounreay, the dumping sites of nuclear waste in the Kara Sea, the sunken submarines Komsomolets and Kursk and Russian nuclear installations (Mayak, Tomsk-7 and Krasjonoyarsk-26) releasing radionuclides to the Russian rivers Ob and Yenisey.

1.1.3 Western European Reprocessing plants

A nuclear fuel reprocessing plant recovers spent nuclear fuel for reuse in fission reactors. The remaining radionuclides are either sent to final storage or released to the environment (UNSCEAR, 1993). In Figure 1.1, the locations of the western European reprocessing plants Sellafield (UK), La Hague (France) and Dounreay (Scotland) are presented. Liquid radioactive wastes from the operation of these plants are discharged via pipelines directly into the Irish Sea, the English Channel and into Scottish coastal waters, respectively. Soluble radionuclides from these sources are subsequently transported further northwards with regional oceanic currents, descriptions of which are given below. Sellafield (formerly Windscale) has been the main contributor to activity releases among the 3 western European reprocessing plants. Maximum discharges of 137Cs and the actinides 239,240Pu and 241Am from Sellafield occurred during the mid to late 1970s (Gray et al., 1995). The introduction of the Site Ion-Exchange Effluent Plant (SIXEP) in 1985 subsequently led to a dramatic reduction in discharges of 90Sr, 134Cs and 137Cs (Gray et al., 1995). Increased throughputs and processing of

residues, led to increased discharges of plutonium and americium during the early-mid 1970s. Discharges then decreased following (i) the operation of a flocculation precipitation facility from the mid 1970s, (ii) the cessation of discharges of concentrates to the sea and (iii) the commissioning of the salt evaporator in 1985 (Gray et al., 1995). Throughout the 1980s and early 1990s (1981-1993), 99Tc was discharged in low levels from Sellafield at a rate of 1.9-6.6 TBq a-1. The 99Tc, that was present in medium active concentrate streams, was held on site during this period, before the commissioning of the Enhanced Actinide Removal Plant (EARP). In 1994, the Enhanced Actinide Removal Plant (EARP) at British Nuclear Fuels (BNFL) Sellafield plant in NW England began operations to treat a backlog of stored wastes (Gray et al., 1995). This resulted in a step increase of 99Tc from a level of approximately 5 TBq a-1 to a level of 72-190 TBq a-1 in the period 1994-1996. The initial impact, in terms of increased activity levels in biota and seawater, of the higher 99Tc discharges from Sellafield was observable in Norwegian coastal environments by 1997 (Brown et al., 1999). The abovementioned releases of 99Tc from western European reprocessing plants compare to a global activity of 99Tc released to the stratosphere in the period 1945-1980 of approximately 140 TBq (Rioseco, 1987).

1.1.4 Other actual and potential sources of radioactivity to the northern marine environment
In addition to these western European reprocessing plants, northern marine waters have also have received an input of different radionuclides from Russian reprocessing plants situated in the tributaries of the Russian rivers Ob and Yenisey (see Figure 1.1). These are namely the Mayak Production Association in the southern Urals, the Siberian Chemical Combine (Tomsk-7) north of the Town of Tomsk and the Krasnoyarsk Mining and Chemical Combine (KMCC). Uncertainty exists in relation to the magnitude of radionuclide inputs from these sources although estimates have been made. For example between 1958 and 1993, routine discharges from the KMCC are estimated to have led to an input of 30-100 TBq of 137Cs into the Kara Sea a level which is of a similar order of magnitude to inputs of Sellafield-derived 137 Cs to the area (Vakulovsky et al., 1995). However, the fact that the prevailing surface marine currents tend to transport contamination away from the Kara Sea in predominantly easterly and northerly directions, suggests that the resultant inputs to the Barents and Norwegian seas have been relatively low. Nonetheless, a potential for significant radionuclide contamination might exist following large accidental releases of radioactivity from these nuclear complexes. Several other sources exist, which also represent potential sources of radionuclides to the Barents and Norwegian seas. Among these are radioactive waste dumped in containers in the Barents and Kara Seas by the Former Soviet Union (FSU), and the sunken submarines Komsomolets in the Norwegian Sea and Kursk in the Barents Sea. The dumping areas and the location of the sunken submarine Komsomolets are given in Figure 1.1. Several investigations have been conducted to detect any leakage from these sources. The Joint Russian Norwegian expert group have been investigating the condition of the contained dumped objects and analysed sediment and water samples at the dump sites. According to Strand et al. (1997), elevated levels of radionuclides in sediments collected in the vicinity of the dumped objects demonstrated that leakage had occurred but that no inputs of radionuclides to the open sea from this source have been detected. The Russian nuclear submarine Komsomolets, following an accident on April 7th, 1989, lies at a depth of 1700 metres, 180 km southwest of Bear Island in the Norwegian Sea. The submarine contains a nuclear reactor and two torpedoes

with nuclear warheads. According to Kolstad (1995) a very small leakage of radioacaesium isotopes may have occurred. The Russian nuclear submarine Kursk sank in the south-eastern, Russian sector of the Barents Sea on 12th August, 2000 in 108 m of water. The submarine was powered by 2 PWR nuclear reactors but information in relation to nuclear weapons systems is currently not available. To date, activity concentration in air, water and sediment in the close vicinity of the Kursk indicate that releases of radioactivity have not occurred. Nonetheless, the radionuclide inventories held on board both the Komsomolets and Kursk have the potential to be released to the water column in significant amounts if the structural integrity of the vessels is lost.

1.2 Prevailing regional marine currents

The continuation of the North Atlantic Current into the English Channel, the Northern Seas (the Irish Sea, the North Sea, the Norwegian Sea, the Barents Sea and the Greenland Sea) and the Polar Basin is shown in Figure 1.2. Atlantic water is defined as water having salinity > 35 (Sakshaug et al., 1994). The North Atlantic Current is a relatively slow moving (< 0.5 knot) surface current and is in principally driven by the north wind (Kiilerich, 1965). The transport of radiocaesium (in the form Cs+) and other soluble radionuclides with the surface circulation pattern from the Irish Sea to the Arctic has been described in many studies, and summarised by Kershaw and Baxter (1995). After releases to the Irish Sea, radiocaesium is in transported with the surface currents northwards, via the North Channel and around the coast of Scotland into the western part of the North Sea (Kershaw and Baxter, 1995). From the point source off the north coast of Scotland, the soluble radionuclides released from Dounreay are transported with the surface currents following the Scottish coast into the western part of the North Sea. According to Guguniat et al. (1996), soluble radionuclides discharged into the English Channel from La Hague are transported south and east of the Sellafield activity in the North Sea. The origin of the water masses in the North Sea are Atlantic water with a high salinity and freshwater from land (Aure, 1998). The North Sea receives Atlantic water from the Norwegian Sea in the north, mainly through the Shetlands and the Faroe Islands, and through the English Channel in the south (Kiilerich, 1965). The circulation pattern of the North Sea is mainly anti-clockwise, in which nearly all water flows via Skagerrak. It is important to stress that this is a climatic average situation, and that changes in this pattern occur (Stre, 1996). Skagerrak is also receiving Chernobyl-derived radiocaesium with the out-flowing low-salinity surface waters from the Baltic (Strand, 1994). Soluble radionuclides are transported further northwards with the Norwegian Coastal Current (NCC) (Kershaw and Baxter, 1995). The NCC, which is generated by the out-flowing surface waters from the Baltic, flows northwards off the Norwegian coast as a wedge within the Atlantic water masses. At the boarder of Russia, the NCC becomes the Murman Coastal Current. At approximately 40 to 45 east, the coastal current is supported with low-salinity water from the White Sea (Sakshaug et al., 1994).

Figure 1.2 : The surface circulation pattern of the Northern Seas (adapted from Aure et al. (1999)).

The continuation of the North Atlantic Current (NAC) is flowing northwards along the continental slope, parallel and west for the NCC (Sakshaug et al., 1994). According to Josefsson (1998), off the southern Norwegian coast and outwards, the NAC and the NCC stay separated. On their way northwards they become partly mixed (Josefsson, 1998). Off Troms, northern Norway, the Atlantic current splits into 2 branches, one branch passes eastwards into the Barents Sea as the North Cape Current and one passes northwards off the western coast of Svalbard as the West Spitsbergen Current (WSC). The North Cape current splits into a southern and a northern branch. Whereas the southern branch joins the NCC eastwards, the northern branch bends under the cold and less salty Arctic water masses and becomes a subsurface current. The main part of the WSC continues northwards along the western coast of Spitsbergen, before it continues through the Fram Strait into the Arctic Ocean further eastwards along the Siberian coast. The less significant part of the WSC bends westwards towards Greenland, joining the south-going East Greenland Polar Current (EGC) as a subsurface current at a depth of 100-300 m. Off Iceland, the EGC becomes a major part of the East-Iceland Current. East of Iceland the latter current joins the north-flowing Atlantic water masses (Kiilerich, 1965).

1.3 Mobility and biological uptake of radionuclides

1.3.1 Mobility
Caesium (atomic number 55) belongs to Group Ia in the periodic table and forms monovalent Cs+ ions in aqueous solutions. Caesium-137 is a conservative radionuclide which means that it behaves as part of its associated water body. This has been used to great effect in marine/oceanographic studies (Jefferies et al., 1973; Baxter et al., 1979; Jefferies et al., Activity per unit mass solid 1982). Caesium has a relatively low Kd ( ) of around 3 x 103 Activity per unit volume liquid for coastal sediments/waters (IAEA, 1985). Although 137Cs is defined as a conservative radionuclide, interaction and subsequent association with the solid phase does occur. This can take place via a number of processes including direct uptake of 137Cs at the sediment-water interface, sedimentation with organic matter either after assimilation or adsorption onto cells, adsorption onto inorganic compounds (e.g. clays, carbonates) or scavenging from solution by iron-manganese oxy-hydroxides, sedimentation with humic matter and direct uptake through assimilation by periphyton or other biota residing on surficial sediments. Caesium+ ions are often sorbed on specific sites located within the wedge zones of illitic crystallites. Caesium fixation (i.e. interlayer collapse of the clay lattice) can then take place leading to the virtually irreversible fixing of the caesium ion within the clay mineral matrix (Hird et al. ,1996). Investigations into the geochemical association of caesium with soils and sediments (e.g. Riise et al., 1990; Wilkins et al., 1984, Wilkins et al. ,1985, Murdock et al. , 1993) have shown a strong association of caesium with the irreversibly bound fraction, which corresponds to an association of radiocaesium with primary and secondary minerals, including illite. The radiocaesium associated with this geochemical phase will not be readily available for biological uptake or remobilisation. However, the radiocaesium molecules associated with exchangeable geochemical phases in marine sediment may be available for uptake by biota and prone to desorption processes. In the Irish Sea, for example, studies (Hunt & Kershaw, 1990; McCartney et al., 1994) confirm that significant inventories of radiocaesium have remobilised from sediment deposits. Strontium (atomic number 38) belongs to Group IIa (alkali earth metals) in the periodic table and forms divalent Sr2+ ions in aqueous solutions. Strontium-90 is a conservative radionuclide having a Kd of 1 x 103 l kg-1 in coastal marine sediments (IAEA, 1985). Strontium-90 appears tends to exist in more easily-exchangeable sites in soils and sediments compared to radiocaesium. Strontium can behave as an analogue for calcium (Blaylock, 1982) which means that it may be involved in biological reactions such as the uptake and formation of exoskeletons in invertebrates - in other words strontium will often become associated with biogenic calcium carbonate prior to precipitation and incorporation in bottom sediments. Radiostrontium tends to be associated with easily exchangeable fractions in soils (and by association sediments) even after long time periods. Such observations, were made by Riise et al. (1990) for soils contaminated after the Chernobyl accident. For a laboratory study using soils dosed with 85Sr, Vidal et al. (1993) demonstrated that the radionuclide was highly soluble. For sandy soil (analagous to sandy sediment) no change in the geochemical phase distribution with time was observed. For sandy loam (analagous to silty, more organic rich sediment) a larger fraction of the 85Sr was associated with organic and carbonate fractions. In the final stage of the experiment a decrease in the exchangeable fraction was observed for the sandy loam. As for 137Cs, sequential extraction data on sediments do not give direct quantitative information on the bioavailability of the radiostrontium to biota. Studies on

waters are more conducive to this. The sequential data suggest that sediments may play an important role in the long-term transfer of radiostrontium to biota because a large fraction of the radionuclide is available in easily exchangeable fractions. Over time the sediments can behave as a reservoir slowly releasing radiostrontium into aqueous phases where it may then be available for uptake. The most stable form of Tc in oxygenated seawater is pertechnetate (TcO 4-), the negatively charged, high valence (VII), oxyanion (Beasley & Lorz, 1986). The pertechnetate ion is soluble with distribution coefficients (Kds - activity per unit mass solid/ activity per unit mass liquid) for sediments low in organic matter rarely exceeding 1-4 (Beasley & Lorz, 1986). In contrast, Kd values for technetium for sediments high in organic matter can be appreciable values of up to 1500 have been reported for this type of sediment (Masson et al., 1989). The surface water masses of the North Sea are oxygen-saturated with a relatively low loading of organic matter and thus technetium is likely to be present predominately as the dissolved pertechnetate ion. It is thus reasonable to assume that Sellafield-derived 99Tc behaves very conservatively in these open water masses and therefore knowledge of the prevailing transport routes in the North Sea is essential in predicting the distribution and fate of 99Tc. Neutron capture by fuel in nuclear reactors progressively builds up atoms of heavy artificial elements referred to as transuranics (Actinide Series). Plutonium (atomic number 94) and americium (atomic number 95) are examples of these elements. Plutonium exhibits four oxidation states (III, IV, V, VI) in the natural environment; americium predominantly exists in the (III) oxidation state. Unlike the other radionuclides considered in this project, the actinides are highly particle-reactive. Despite this strong association with the particulate phase, fractions of total Pu releases/inputs may be transported over considerable distances. Ratios consistent with a significant input from BNFL Sellafield, for example, have been determined at location as remote as the Barents Sea (Kershaw & Baxter, 1995; Grttheim, 1999). The IAEA (1985) recommended Kd value, in coastal waters, for plutonium is 1 x 105 and for americium is 2 x 106. The plutonium oxidation states have a major influence on its Kd values, i.e. Pu (III & IV) = 1 x 106 and Pu (V & VI) = 1 x 104. Field measurements represent the properties of the particular mixture of oxidation states present (Nelson & Lovett , 1978). In open oceanic environments, Pu appears to be removed from biologically-mediated scavenging processes and released back into solution to form a subsurface maximum (Sholkovitz, 1983). Nonetheless, a small portion of originally-dissolved Pu is likely to reach deep ocean beds after it becomes associated, for example, with larger biogenic particles. Direct inputs of waterborne particulate and colloidally-bound actinides may also occur to studied sea areas before deposition to the sea bed occurs. Sequential extraction experiments (Aston et al. , 1981; Aston & Stanners, 1981; Cook et al., 1984; Wilkins et al., 1984; McDonald et al. , 1990; McDonald et al., 1992; Murdock et al., 1993; Murdock, 1995) have shown the importance of the organic and sesquioxide fractions in the geochemical phase association of plutonium in marine/freshwater sediments and soils. The concentration and speciation of plutonium appears to be related to the redox chemistry of iron (Sholkovitz, 1983). This is particularly relevant in freshwater lakes where plutonium in sediments can be dissolved and mobilised if the sediments became anoxic and Fe and Mn-reducing. The phase association of americium is less clear. Wilkins et al. (1984) reported that the carbonate fraction was important in an estuarine sample but that the organic phase was dominant for a (estuarine) saltmarsh sample. Although 241Am exists primarily as a trivalent ion in solution, it may still form complexed species which behave analogously to plutonium (Murdock et al. , 1993). Early diagenetic reactions appear to allow the release of small fractions of the sediment Pu inventory back to the water column. For example, Cook et al. (1997) estimated an annual loss of over 1 TBq a-1

dissolved phase 239,240Pu, consisting mainly of remobilised-Pu, from the North Channel in the Irish Sea in the early 1990s.

1.3.2 Biological uptake

On reaching Norwegian coastal waters, radionculides will be assimilated, to varying extents, by biota. Uptake of radionuclides can occur directly from the water column via adsorption (e.g. through gill membranes in the case of fish) or indirectly through the ingestion of contaminated prey species or particulates via adsorption through the gut and intestine (e.g. for higher trophic levels). The degree of uptake is dependent on the physico-chemical form of the radionuclide ranging from cations dissolved in water to radionuclides forming organic complexes bound within living tissue. In its simplest terms, the bioaccumulation of a radionuclide is often expressed as a concentration factor, CF, defined as the ratio of the radionuclide activity concentration in biota (normally Bq kg-1, wet weight) to that in sea water (Bq l-1). The CF term relates to a situation whereby abiotic and biotic compartments have reached equilibrium. This is often not the case in the real environment where ambient, abiotic concentrations may change significantly in time and space owing to complex temporal inputs of radionuclides or variability in the parameters influencing activity concentrations in abiotic compartments, e.g. changes in suspended load, salinity etc. Typical CFs for Cs, Sr, Pu, Am are presented in Table 1.1.
Table 1.1 : IAEA (1985) recommended values for Concentration Factors
Organism Fish Crustaceans Mollusca (excluding cephalopods) Cs 100 30 30 Concentration factors Sr Pu 2 40 2 300 1 3000 Am 50 500 20000

Certain species of biota exhibit very high uptake of 99Tc. Concentration factors for selected species (the selection based on the basis of their importance in the human diet and/or high uptake of 99Tc) in the Irish Sea after the initial operation of EARP, are listed in Table 1.2.

Table 1.2 : Examples of Concentration Factors (activity per unit mass (wet weight) of biota/activity per unit mass of water) for selected biota in the Irish Sea in 1995.
Organism Seaweed Mussels Lobster Lobster Norwegian lobster Norwegian lobster Description/species Fucus vesiculosus 1 Mytilus edulis Homarus gammarus -abdomen muscle 2 Homarus gammarus -green gland 2 Nephrops norvegicus abdomen muscle 2 Nephrops norvegicus -Hepatopancreas 2 CF 1.19 0.41x105 500 720 6.5 x 105 970 2300 Reference Smith et al. (1997) McCartney & Rajendran (1997) Busby et al. (1997) Busby et al. (1997) Busby et al. (1997) Busby et al. (1997)

1 : CF dry weight 2 : CF to body part

Certain species of brown seaweeds (e.g. Fucus vesiculosus) concentrate 99Tc to a high degree. In the Irish Sea, CFs (based on dry weight), for Fucus vesiculosus, in excess of 1 x 105 (Smith et al., 1997) have been measured. Other species of brown seaweed also exhibit high concentration factors. Concentrations of 99Tc Fucus serratus, sampled in the Irish Sea in 1995, were about 72 % of the concentrations observed in Fucus vesiculosus (McCartney & Rajendran, 1997). Uptake of 99Tc by the common lobster and the Norwegian lobster is also significant.

1.4 Traditional impact assessments

Radiological environmental impact assessments normally focus upon the transfer of radionuclides to man and effects of radiation exposure on individual humans. If no data concerning radionuclide concentrations in environmental media exist, an assessment will begin with a study of the transfer of radionuclides through the environment in order to predict the resultant concentrations in human food-stuffs and surroundings. Alternatively monitoring data can be used directly as input for dose calculation, removing the need to use environmental transfer models. Approaches then vary depending on whether the assessment is concerned with (i) calculation of exposure to those members of the public, who by result of their diet or living habits are exposed to the highest levels of radiation from a selected source a so called critical group or (ii) calculation of doses to the world population or subsets of that population, i.e. collective dose assessment. The critical group approach requires a collation of data relating to dietary intake and living habits. These data are then used to calculate internal doses, which partly involves the application of factors to convert from Bq intake to committed effective dose (e.g. Phipps et al., 1991), and external doses, which partly involves the application of a simple dose conversion coefficients mapping a gamma air kerma rate to an effective dose equivalent (e.g. ICRP, 1996). Radiation doses received by humans can then be evaluated in terms of potential effects. At very high doses, such as those that may arise in nuclear accident near-zones, deterministic effects e.g. death, severe organ damage etc. may be of prime concern. Under more normal dose ranges, such as those measured in European coastal areas, only a stochastic effect can be derived. This normally relates to the probability (risk) of individuals within a population developing a cancer within a defined time period.

As described above, radiological protection frameworks have traditionally been firmly focused on the protection of man. This has arisen, primarily because the advisory body on such matters, that is the International Commission on Radiological Protection (ICRP), has maintained a strong bias towards human health issues stating the view that if man is adequately protected then other living things are also likely to be sufficiently protected (ICRP, 1977). More recently a caveat has been added (ICRP, 1991) that individual members of non-human species might be harmed but not to the extent of endangering whole species or creating imbalance between species. In most cases this tenet appears to have sufficed in protecting the environment from observable harm. This is largely due to the fact that dose limits to man are set at a low level where effects at even the most vulnerable part of a food web are unlikely to be seen. However, it has become increasingly evident that problems do exist in the extension of the current tenets of radiological protection to environmental radiation protection. The need for the development of a new system, which can be used to explicitly assess impacts of radioactivity on flora and fauna, has arisen for several reasons : (a) The ICRPs view is not valid for all situations. Such a situation could exist where pathways to man do not exist. In another example, it has been shown (Pentreath, 1998) that for deep sea disposal (although no longer practised) could result in a harmful dose to biota whilst still maintaining doses to man well below the recommended dose limits. (b) Statements relating to environmental protection have been introduced into the contents of international conventions (e.g. OSPAR) and the legislation of individual countries. At present there is no internationally-accepted methodology for performing an environmental impact assessment for radioactivity and thus there are no means of showing that the environment is, in fact, being protected from ionising radiation. This is clearly not good practice and leads to the undermining of public confidence. (c) There is inconsistency with the standards for other hazardous materials such as heavy metals and organic chemicals. Here, specific environmental protection criteria are applied, e.g. concentration standards in specific vulnerable biota. A more consistent, integrated approach is required, whereby the total environmental impact from a site discharging both radioactive and non-radioactive substances can be assessed. In order to develop a coherent and logical environmental impact assessment methodology for ionising radiation, a framework, within which models can be applied and results analysed, is prerequisite. A number of components that could form the basis for this type of system, have been suggested by Pentreath (1999). These include a set of reference organisms - clearly not all organisms can be studied necessitating a selection procedure. a set of quantities and units to express a dose to biota. In current practice doses are expressed in Grays per unit time, which clearly excludes relative biological effects arising from radiation type. a reference set of dose models for a number of reference flora and fauna. Calculation methodologies exist allowing the calculation of doses to organisms with varying geometries, e.g. Woodhead (1979). Consensus is required in adapting these algorithms for use within a framework. a set of dose-effects relationships for reference organisms which could include data from low exposure, e.g. cytogenetic effects to high exposure, e.g. lethal effects, situations.

1.5 Project objectives

The main aim of the project was to obtain information about the vulnerability of the Arctic marine environment in relation to different radionuclide release scenarios and to make recommendations for future monitoring programmes. Basic knowledge of the controlling processes on uptake already exists. This project aims to build on this understanding and to focus on factors considered to be relevant for Arctic environments. This will be achieved through the following objectives : (1) To identify and quantify the key parameters that control uptake and accumulation of anthropogenic radionuclides in marine biota through field investigations and laboratory experiments. (2) To collate information relating to transfer (fluxes) of radionuclides though marine food-webs (3) To develop new models (doses to biota and human radiological assessment) using the information from field and laboratory studies.

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McDonald, P., Cook, G.T., Baxter, M.S. & Thomson, J.C. (1990). Radionuclide transfer from Sellafield to south-west Scotland. Journal of Environmental Radioactivity, 12, 285-298. McDonald, P., Cook, G.T., Baxter, M.S. & Thompson, J.C. (1992). The terrestrial distribution of artificial radioactivity in south-west Scotland. The Science of the Total Environment, 111, p.59-82. Murdock, R.N., Johnson, M.S., Hemingway, J.D. & Jones S.R. (1993). Physicochemical characteristics of radionuclides associated with sediment from a contaminated fresh water stream. Environmental technology, 14, pp. 639-648. Murdock, R.N. (1995). The use of salt marsh sediment cores to reconstruct historical pollution profiles in the Mersey and Ribble Estuaries, UK. Postdoctoral Research project, Department of Environmental and Evolutionary Biology, University of Liverpool. Nelson, D.M. & Lovett (1978). Oxidation states of plutonium in the Irish Sea. Nature, 276, pp.599-601. Pentreath, R..J. (1998) Radiological protection criteria for the natural environment. Radiation Protection Dosimetry, 75, 175-179. Pentreath, R.J. (1999). A system for radiological protection of the environment: some initial thoughts and ideas. J. Radiol. Prot. 19(2), 117-128. Phipps, A.W., Kendal, G.M., Stather, J.W. & fell, T.P. (1991). Committed Equivalent organ doses and committed effective doses from intakes of radionuclides (National Radiation Protection board, Chilton, UK, NRPB-R245. Rioseco, J.L. (1987). Technetium-99 : Radioanalytical and radioecological studies. Department of Radiation Physics, Lund University. Riise, G., Bjornstad, H.E., Lien H.N., Oughton D.H. & Salbu, B. (1990). A study of radionuclide association with soil components using a sequential extraction procedure. Journal of radioanalytical and Nuclear Chemistry, Articles, 142, pp.531-538. Sakshaug, E., Bjrge A., Gulliksen, B., Loeng, H., Mehlum, F. Eds. (1994). kosystem Barentshavet (in Norwegian). Oslo : Norges forskningsrd, Universitetsforslaget. Sholkovitz, E.R. (1983). The geochemistry of plutonium in fresh and marine water environments Earth Review, 19, pp.95-161. Science

Smith, V., Ryan, R.W., Pollard, D., Mitchell, P.I. & Ryan, T.P. (1997). Temporal and geographical distributions of 99Tc in inshore waters around Ireland following increased discharges from Sellafield. Radioprotection Colloques, 32, 71-77. Strand, P. (1994). Radioactive fallout in Norway from the Chernobyl accident. Studies on the behaviour of radiocaesium in the environment and possible health impacts. Strlevernrapport 1994:2. sters, Norwegian Radiation Protection Authority. Strand P., Nikitin A.I., Lind B., Salbu B., Christensen G.C., (1997). Dumping of radioactive waste and investigation of radioactive contamination in the Kara Sea. Results from 3 years of investigations (1992-1994) in the Kara Sea. Joint Norwegian-Russian Expert Group for investigation of radioactive contamination in the Northern Areas. sters: Norwegian Radiation Protection Authority, NRPA, 1997. Strand, P., Balonov, M., Aarkrog, A., Bewers, M.J., Howard, B., Salo, A & Tsaturov, Y.S. (1998). Chapter 8 : Radioactivity. In : AMAP Assessment Report : Arctic Pollution Issues. Arctic Monitoring and assessment Programme (AMAP), Oslo, Norway, pp. 525-620. Stre, R. (ed.) (1996). Miljrapport 1996 (in Norwegian). Fisken og havet, Srnr. 2-1996. Bergen : Havforsningsinstituttet.

UNSCEAR (1988). Sources, effects and risks of ionising radiation. The United Nations Scientific Committee on the Effects of Atomic radiation. New York. UNSCEAR (1993). Sources and effects of ionising radiation. The United Nations Scientific Committee on the Effects of Atomic radiation. UNSCEAR 1993 Report to the General Assembly with scientific annexes. New York: United nations, 1993. Vakulovsky, S.M., Kryshev, I.I., Nikitin, A.I., Savitsky, T.V., Malyshev, S.V., Tertyshnik, E.G. (1995). Radioactive contamination in the Yenisey River. Journal of Environmental Radioactivity, 29 (no 3), pp.225-236. Vidal, M., Tent, J., Llaurado, M. & Rauret, G. (1993). Study of the evolution of radionuclide distribution in soils using sequential extraction schemes. Journal of Radioecology, 1, pp.49-55. Wilkins, B.T., Dodd, N.J., Green, N., Major, R.O. & Stewart, S.P. (1984) . The disposition of caesium-137, iodine-129, ruthenium-106, strontium-90, americium-241 and plutonium in estuarine sediments and coastal soils. In : Proceedings of the International Seminar on the Behaviour of radionuclides in Estuaries, Renesse, The Netherlands, 17-20th September 1984, pp.55-70. Wilkins, B.T., Green, N., Stewart, S.P. & Major, R.O. (1985). Factors that affect the association of radionuclides with soil phases. In : Speciation of fission and activation products in the environment, eds R.A. Bulman & J.R. Cooper. Elsevier Applied Science Publishers, London and New York, pp.101-113. Woodhead, D.S. (1979). Methods of dosimetry for aquatic organisms. In : Methodology for assessing impacts of radioactivity on aquatic ecosystems. IAEA Technical Report Series No. 190. International Atomic Energy Agency (IAEA, Vienna) 43-96.

2. Methodology
Authors : Justin Brown, Anne Liv Rudjord, Bjrn Lind: Norwegian Radiation Protection Authority Brit Salbu: Agricultural University of Norway Gordon C.Christensen, Elisabeth Strlberg: Institute for Energy Technology Lars Fyn: Norwegian Institute of Marine Research Ivan Kryskev, Tatiana Sazykin: SPA Typhoon

2.1 Field work Barents Sea expedition January-February 1999

Samples were taken during an expedition to the Barents Sea on board the research vessel F/F Johan Hjort. The samples taken in the Russian sector of the Barents Sea (roughly east of longitude 300 E) were collected in the period 27/01/1999 09/02/1999 and the samples (from 3 locations) taken in the Norwegian sector of the Barents Sea in the period 10/02/1999 23/02/1999. The period between sampling was normally 1-2 days. For the 7 sampling stations in the Russian Sector, filtered surface seawater (0.45 m and 1 m) was collected for 99Tc, 137 Cs and 241Am/Pu analyses. At 2 stations sediment profiles were also sampled and at a further 2 stations detailed studies were conducted which included collection of surface and bottom waters, collection of waters for analyses of 90Sr, fractionation of waters (10 kDa) for Pu/Am and collection of sediment cores. In addition to the collection of water and sediment, biota samples were also taken including cod, polar cod, shrimp, flounder and king crab. The sample locations are shown in Figure 2.1.

Figure 2.1 : Sampling locations in the Barents Sea from the sampling expedition in January/February 1999. Sampling locations number 1-10.

2.2 Sampling and pre-treatment of samples Barents Sea expedition January-February 1999
2.2.1 Sampling of biota and sediment
Sediments were originally collected using a box-corer and a surface grab. Two profiles were removed from each box by slowly inserting PVC tubes of 100 mm diameter to a depth of 1525 cm. All sediment samples were frozen onboard ship following sampling. Biota samples were taken using a bottom trawl. The locations roughly corresponded to those positions where water and sediment samples were taken although deviations of up to several hundred metres were introduced owing to the nature of the sampling method.

2.2.2 Pretreatment of sea water during field-work

The sampling and pre-treatment for the determination of 137Cs in seawater, involved the pumping of water (up to several hundred litres) directly through a system consisting of 3 chambers. The first chamber contained a 1 m pre-filter, the next 2 in series contained cartridges coated in Cs-sorbent (Cu2Fe(CN)6). A flow-meter mounted at the end of the rig allows the volume of water passing through the system to be calculated The sampling of seawater for 99Tc analyses simply involved pumping 50 litres of water into canisters ready for transportation. For the determination of actinides in sea water, samples (approximately 200 l) were pretreated by adding a 242Pu spike and co-precipitating Pu with Fe hydroxide following the addition of Fe (II) solution and adjusting pH to 9.5. The precipitate was isolated, by decanting the liquid, before transferring to small canisters and transporting to the laboratory.

2.2.3 Ultrafiltration of Pu isotopes

At 2 sampling locations, seawater samples were fractionated using hollow fibres (Amicon membrane, cut-off 10 kDa) before the determination of Pu isotopes.

2.3 Laboratory studies

Kinetic tracer and sequential extraction experiments were conducted at AUN. Further details are provided in Chapter 4 of this report. Uptake experiments on phytoplankton were conducted by IMR. Further details are provided in Chapter 5.

2.4 Analyses of field samples from Barents Sea 1999 expedition

2.4.1 -emitting radionuclides
Sorbents (seawater), sediments and biota samples were dried and, in the case of Cs-sorbents, ashed before analyses. The analyses for gamma emitters, including 137Cs involved the use of HPGe detectors (resolution = 1.7-2.0 keV, efficiencies in the range of 10-55 %). Further details can be found elsewhere (Strand et al., 1997). Sediment profiles from stations 3 and 6 were determined for -emitting radionuclides by AUN. The profiles were sliced in 2 cm sections. 137Cs in dried sediments (105C) are determined using gamma spectrometry with Ge-detectors (Canberra, 20% efficiency and 1.6 keV resolution at 1332 keV) interfaced to a PC equipment with Genie PC software (Canberra). Determinations of -emitting radionuclides from Stations 5 and 7 were made by IFE.

2.4.2 -emitting radionuclides

Seawater samples from all stations were measured for 99Tc at the NRPA. The method for 99Tc determination involves the use of ion chromatography and solvent extraction using 99mTc as a yield monitor. Levels of 99Tc are determined using a low background anti-coincidence beta counter. The combined uncertainty (1 standard deviation) lies between 5 and 8 % for both biota and seawater. The detection limit for seawater (50 l) is 0.14 Bq m-3 and for biota approx. 0.6 Bq kg-1. Further details can be found elsewhere (Kolstad et al., 1999). Seawater samples from Stations 3 & 6 were measured for 90Sr at AUN. Sr-analysis was based on precipitation with Fe-hydroxide, performed on board the ship. The concentration of 90Sr was determined by measuring the erenkov-radiation of 90Y by Quantulus low level liquid scintillation counter after the separation of 90Y (oxalate precipitation and nitrate precipitation using fuming nitric acid using low background -counter or Quantulus). The concentration of 90 Sr in sediments (at AUN) was determined by measuring the erenkov-radiation of 90Y by Ouantulus low-level liquid scintillation counter after ashing, digestion in aqua regia and liquid-liquid extraction with 5% HDEHP. Sr-85 is used as a yield monitor. Selected sediment samples from Stations 5 & 7 were analysed for their 90Sr content at IFE. Analysis was based on the fuming nitric acid method and determinations made by counting samples of yttrium oxide on low background anti-coincidence beta counters. The 90Sr content of biota samples (12 in total) was also determined at IFE using a related radiochemical procedure. More detail can be found elsewhere (Strand et al., 1997).

2.4.3 -emitting radionuclides

For Pu determinations at the NRPA, samples (precipitate from water, aqua regia extracts from sediment and biota) were separated using (i) solvent extraction (TIOA/xylene solution) and (ii) ion exchange chromatography. The Pu was electrodeposited on stainless steel planchettes and measured for -emissions using semiconductor silicon detectors. Further details can be found in Strand et al. (1997). IFE determined the Pu content of sediments from stations 5 and 7 using standard radiochemical techniques.

Plutonium-239, 240 in sediments was determined by AUN using Inductively Coupled Plasma Mass Spectrometry (ICP-MS, Perkin Elmer ELAN 6000) after ashing, digestion in aqua regia and standard radiochemical separation on ion-exchange columns. Pu-242 is used as yield monitor.

2.5 Human and biota dosimetric models

In order to assess the impact of radionuclides to man and the environment, dosimetric models have been used. The models have been adapted specifically for use in the northern seas using input data from this project and historical data archived in Russian institutes. The methodology for dose calculation for biota/hydrobiants is presented in Chapter 6 (both TYPHOON and NRPA methodology). The process involves the application of , and internal and external dosimetric models to (i) real data from historical data sets and those data produced in the present project (presented in the Results Section Chapter 3) and (ii) modelled data derived from release scenarios. Doses to biota are calculated in absorbed dose (Gy) per unit time. The methodology for the determination of doses to man is presented in more detail in Chapter 7. The process adopted by TYPHOON involves a collation of historical activity concentration data (presented in the Results Section Chapter 3) and the application of modelled data derived from release scenarios. Following this, calculations that account for dietary information or production statistics (Chapter 7) using dose conversion factors are applied in order to calculate committed effective doses and collective doses.

References
Kolstad, A.K., Lind, B. & Rudjord, A.L. (1999). Kalibreringsrutiner og metodebeskrivelse av StrlevernRapport 1999:12. Norwegian Radiation Protection Authority, sters, Norway, pp 31.
99

Tc-analyser.

Strand P., Nikitin A.I., Lind B., Salbu B., Christensen G.C., (1997). Dumping of radioactive waste and investigation of radioactive contamination in the Kara Sea. Results from 3 years of investigations (1992-1994) in the Kara Sea. Joint Norwegian-Russian Expert Group for investigation of radioactive contamination in the Northern Areas. sters: Norwegian Radiation Protection Authority, NRPA, 1997.

3. Radionuclide activity concentrations in the environment

Authors :

Justin Brown, Anne Liv Rudjord, Bjrn Lind: Norwegian Radiation Protection Authority
Brit Salbu: Agricultural University of Norway Gordon C.Christensen, Elisabeth Strlberg: Institute for Energy Technology Lars Fyn: Norwegian Institute of Marine Research Ivan Kryshev, Tatiana Sazykin: SPA Typhoon

This chapter has been split into 3 parts. In Section 3.1 data compiled through literature review is presented. These data are useful both in terms of placing the radionuclide activity concentrations determined in the course of the present study in the context of historical trends and as input data sets for dose rate calculations performed in Chapters 6 (Ecological dosimetry models) and 7 (Dose assessment for human populations). In the second part of the results chapter, Section 3.2, the results from the Barents Sea expedition, 1999, are reported and discussed. These data have also been used for further interpretation in the context of the themes covered in Chapters 4 and 6. In Section 3.3 data are presented for 137Cs and 99Tc in seaweed for Norwegian coastal water sites.

3.1 Collation of data

An updated data base on the radionuclide concentration in water, bottom sediments and biota of the Arctic Seas is presented in Tables 3.1-3.3 (for the period 1991-1998) (Environmental Radioactivity in the Arctic 1993, 1995, 1997, 1999; Strand et al., 1993, 1994, 1997; Vakulovsky et al., 1993; Nikitin et al., 1994, 1997; Holm, 1994; Matishov et al., 1994; Chumichev, 1997; AMAP, 1998; Mitchell et al, 1998; Brown et al, 1999a; Radioactive Contamination in the Russian Arctic, 1999). The data collation was performed by TYPHOON.
Table 3.1. Concentration of radionuclides in the surface waters of the Arctic Seas (1991-1998), Bq/m3
Sea Barents Kara Norwegian North Greenland White Bering Laptev Chukchi
90

Sr 4.0 1.0 5.1 2.0 3.2 0.7 2.0 0.2 6.8 2.5 1.8 0.8 5.2 1.5 2.1 1.0

137

Cs 5.8 1.5 6.2 1.6 6.7 3.6 8.3 6.1 7.0 1.0 10.0 2.0 1.6 0.5 5.0 4.0 2.5 0.6

239,240

Pu 0.005 0.003 0.004 0.002 0.007 0.004

241

Am 0.0007 0.0003 0.0008 0.0004 0.001

99

Tc 0.15 0.14 5.0

210

Po

1-2

Table 3.2. Concentration of radionuclides in the bottom sediments of the Arctic Seas (1991-1998), Bq/kg d.w.
Sea Barents Kara Norwegian
90

Sr 0.32 0.15 1.5 1.3 3.5

137

Cs 8 3 15 6 1.9

239,240

Pu

241

Am

99

Tc

210

Po

4 0.38 0.23 0.003 0.15 0.10 0.0008 0.5 20

Table 3.3. Concentration of radionuclides in the biota of the Arctic Seas (1991-1998), Bq/kg
Biota/Sea Fish (f.w.) Barents Kara Norwegian North Greenland Cod Barents Norwegian Saithe Barents Norwegian North Haddock Barents Norwegian North Shrimps (f.w.) Barents Norwegian Lobster (f.w.) Norwegian Mussels (f.w.) Norwegian Kamchatka crab (f.w.) Barents Benthos (f.w.) Barents Kara Norwegian Seaweed (d.w.) Barents Kara Norwegian Greenland Minke whale (f.w.) Barents Norwegian Greenland seal (f.w.) Greenland White
90

Sr

137

Cs

239,240

Pu

241

Am

99

Tc

210

Po

0.02 0.01 0.03 0.01

0.84 0.63 0.56 0.47 0.48 0.17 0.22 0.05 0.31 0.07 0.9 0.4 0.48 0.03 0.38 0.03 0.45 0.05 0.25

<0.006

0.03

0.004

0.45 0.15 0.38 0.08 0.15 3.9 2.4 0.15 0.03 0.5 0.0007 0.007 0.0005 0.02 26 12 0.6 17 60

0.75 2.6

0.5 0.4 0.14 0.06 4.2 0.3 3.0 2.8 1.0 0.6 4.0 2.2 1.7 0.7 14 0.5 1.5 0.3

0.18 0.10

0.024 0.065 0.05 0.041 0.008

8 4.1

0.18 0.16 0.045 0.1 0.02

0.008

45

0.35

0.9 0.5 5.7 1.0 0.0013 0.14 0.04

1.2 0.3 3.9 2.5

0.004 0.001 0.01 0.008

0.4 0.12 0.61 0.25

3.2 Results from the Barents Sea expedition 1999

3.2.1 Radionuclides in seawater
3.2.1.1 Technetium-99 in seawater Data are presented showing levels of 99Tc in the surface waters of Barents Sea in February 1999 (Fig. 3.1).

Figure 3.1 : Levels of 99Tc (Bq m-3) in the surface waters of the Barents Sea - February 1999. Activity concentrations at each location are based on single measurements. Total uncertainties (1 standard deviation) are approximately 8 %. The arrows represent the major currents in the area responsible for the advection of Sellafield-derived, conservative radionuclides into Arctic waters.

An average of 0.15 Bq m-3 99Tc has been derived for the period 1991-1998 (Table 3.1). Other estimates (Brown et al., in press) report that regional background for the early 1990s probably fell in the range 0.2-0.4 Bq m-3. It is clear from this information that elevated concentrations, above these estimated regional background levels for earlier years, are observed within a few hundred kilometres of the northern coasts of Norway and the Kola Peninsula in 1999. At open sea locations in the central Barents Sea, activity levels are lower, resembling the estimated regional background for the early 1990s. The reason for the increase in activity concentrations at some locations is connected to new inputs of 99Tc to the Arctic marine environment following the increased discharges from EARP at Sellafield in 1994.

The eastward transport pathway, for conservative radionuclides en route from Western European reprocessing plants, as described by Kershaw & Baxter (1995), appears to be clearly delineated by the 99Tc levels. Towards the central parts of the Barents Sea, Atlantic water bearing relatively low levels of 99Tc predominates, whereas, further south, sea water originating from the Norwegian Coastal Current (NCC), bearing enhanced levels of 99Tc flows into the Southern Barents Sea following the Nordkapp Current (Murman Current further east). The information so-far derived from the development of the 99Tc contamination distribution following the operation of EARP from the present study and early work (e.g. Leonard et al., 1997; Brown et al., 1999b) is consistent with existing knowledge pertaining to the surface circulation pattern of the North Atlantic and adjacent seas. 3.2.1.2 Caesium-137 in seawater Activity concentrations of 137Cs in the Barents Sea from the expedition of 1999 are shown in Figure 3.2. Levels of 137Cs range from 2.8 0.13 to 4.0 0.17 Bq m-3. Although this range is small, the low uncertainty associated with measured activity concentrations (approx. 5 % for 1 ) means that differences in the measurement values are significant. Maximum activity concentrations were measured at over 100 km from the coast. Lowest activity concentrations were measured at near coastal sampling locations and areas in the open Barents Sea at distances >200 km from the coast. The spatial pattern of 137Cs contamination is similar, albeit with lower contrast between levels, to that observed for 99Tc. An inspection of salinity data shows that the highest measured activity concentrations are associated with salinities in the range 34.5 to 34.8 . The low 137Cs activity concentrations are associated with salinities above and below this range. These observations are consistent with what is known with regards to the sources of radiocaesium to the area and the nature of the prevailing marine currents. Radiocaesium in Arctic waters is mainly derived from global fallout, reprocessing plants in western Europe (in particular BNFL Sellafield) and the Chernobyl accident (Strand et al., 1998). Radiocaesium inputs from BNFL Sellafield enter the Barents Sea primarily via the Norwegian Coastal Current as described above for Sellafield-derived 99Tc. It should be noted that at the present time a large fraction of Sellafield-derived 137Cs is likely to be a remobilised component of the discharges that took place in the earlier years of plant operations. In the case of inputs from the Chernobyl accident, a key source of 137Cs is the Baltic Sea, which receives river runoff from highly contaminated terrestrial environments. The outflow of relatively low salinity waters from the Baltic Sea combine with water in the Skaggerak and join the NCC in its southern extremities. Contaminants entering the Barents Sea via the NCC will tend to be transported close to the coast. Water masses carrying relatively high concentrations of 137Cs in the Murman Current will mix with relatively uncontaminated freshwater very near to the coast and relatively uncontaminated Atlantic water in more central parts of the Barents Sea. In both cases this will lead to a reduction of the contaminant levels observed at these locations below those levels observed on the main trajectory of the Murman Current. The activity concentrations of 137Cs measured in 1999 are consistent with the decrease in the levels of this radionuclide in this area, recorded elsewhere (Strand et al., 1998). A peak of 50 Bq m-3 137Cs was measured in the Barents Sea in the early 1980s following a period of high release from BNFL Sellafield several years earlier. Following a decrease in 137Cs discharges from Sellafield by over 2 orders of magnitude (between the mid 1970s and 1990s) and a decline in 137Cs inputs from land runoff, following the Chernobyl accident, the levels of 137Cs in the Barents Sea had fallen to 4-8 Bq m-3 in 1994 consistent with the value of 5.8 1.5 Bq

m-3 recorded in Table 3.1 for the period 1991-1998. The decline in activity concentrations appears to have continued up to 1999.

Figure 3.2 : Levels of 137Cs (Bq m-3) in the surface waters of the Barents Sea - February 1999. Activity concentrations at each location are based on single measurements. Total uncertainties (1 standard deviation) are approximately 5 %.

3.2.1.3 Bottom water samples 99Tc and 137Cs Two bottom water samples, from Station 3 and Station 6 were also analysed for 99Tc and 137 Cs. These data are presented in Table 3.4 along with data for surface waters for comparison purposes..

Table 3.4 : 99Tc and 137Cs activity concentrations (Bq m-3) in surface and bottom sea water samples from Stations 3 and 6 in the Barents Sea.

Station 3 (surface) 3 (bottom) 6 (surface) 6 (bottom)

Depth (m) 0 132 0 230

Salinity 34.63 34.64 34.80 34.87

99

Tc (Bq m-3) 0.97 0.08 0.54 0.04 0.54 0.04 < 0.01

137

Cs (Bq m-3) 3.65 0.17 3.41 0.17 3.35 0.13 2.5 0.13

These data are interesting because the 99Tc activity concentrations in the upper water column are distinctly higher than those in the lower part of the water column. This is despite the fact that, at both locations, there was little difference in the salinity recorded in top and bottom waters. The water columns at Stations 3 and 6 were not vertically stratified and apparently not formed from more than one water mass. The activity concentrations of 137Cs, in contrast, appear to be more uniform with depth. Earlier data pertaining to 137Cs activity concentrations, from the 1980s, for cross sections between Bjrnoya and Fugloya (20 E, Western Barents Sea) (Kershaw & Baxter, 1995) showed some variation in activity concentrations with depth but such variations could largely be explained by the mixing of distinctive water masses. Results from work conducted in the summer of 1995 (Grttheim, 1999) show a fairly uniform 137 Cs activity concentrations with depth for a number of locations in the Barents Sea. On initial inspection, a similar pattern of homogeneous 99Tc activity concentrations with depth, for a selected water mass, might be expected because (i) the behaviour of 137Cs and 99Tc under normal marine conditions is similar i.e. conservative and (ii) the physical processes leading to the advection and dispersion of both radionuclides, e.g. transport by marine currents, are identical. However, differences are introduced by the fact that the component of activity concentration attributable to global fallout was and is much higher for 137Cs than for 99Tc. Caesium-137 activity concentrations in the Barents Sea area arising from global fallout in the 1980s were probably in the range of 3-6.2 Bq m-3 (Kershaw and Baxter, 1995) compared to the actual measurements (all sources) from the Bjrnoya-Fugloya transect (1981-1989) in the range 2-47 Bq m-3. An activity concentration of 0.005-0.01 Bq m-3 from global fallout is more typical for 99Tc. This value is derived by applying a concentration factor of approximately 1 x 105 typical of 99Tc in Fucus seaweeds (Brown et al., 1999) to an activity concentration of 0.51 Bq kg-1 99Tc, representative of Fucus growing in areas contaminated by global fallout only (Holm et al., 1983). This compares to the activity concentrations measured in the present study of 0.2-1.1 Bq m-3 99Tc. Clearly the global fallout component of 99Tc activity concentrations is small. The majority of radiocaesium deposition, which occurred in the period 1955-1966 (Strand et al., 1998), will have become well dispersed (laterally and vertically) in the northern seas by the 1980s and therefore a uniform activity distribution of global-fallout derived 137Cs in the vertical plane, for selected water masses, might be expected. In addition, the continuous discharges from BNFL Sellafield and La Hague in the 30 years or so prior to the sampling in the 1980s would also be well dispersed and add to the background activity concentrations above which any new signal would need to be distinguished. The global fallout component of 99Tc in Arctic waters has been negligible in comparison to inputs from W European reprocessing plans. Although low-levels of 99Tc were released from La Hague and Sellafield in the 1980s and early 1990s adding to regional background activity concentrations, any new significant inputs to the regional marine system should be clearly observable. A step increase of 99Tc discharges from a level of approximately 5 TBq a-1 to a level of 72-190 TBq a-1 in the period 1994-1996 occurred following the commissioning of

the Enhanced Actinide Removal Plant at Sellafield, providing exactly this type of situation. This has resulted in a relatively simple spatial distribution pattern arising from the dominant influence of a single source, i.e. Sellafield, for 99Tc as oppose to the rather convoluted spatial distribution pattern, arising from the influence of multiple sources of similar magnitude, seen for 137Cs. The available data suggest that the dispersion and turbulent mixing of 99Tc in the vertical plane of individual water masses, following release from Sellafield and transport to the North, has occurred to a limited extent. More data are required to establish whether the representative of the larger system. 3.2.1.4 Strontium-90 in seawater
99

Tc data derived from this study are

Strontium-90 in seawater has was determined at 2 stations only. At Station 3 an activity concentration of 1.65 0.17 Bq m-3 was determined and at Station 6 an activity concentration of 1.76 0.18 Bq m-3 was determined. These values are approximately 50 % of the average activity concentration derived for the period 1991-1998 (Table 3.1). The limited number of samples taken in the present study, render any explanations given with regards to the apparent decline in activity concentrations highly speculative. Nonetheless the data are consistent with our knowledge of the behaviour of 90Sr in marine systems. The sources of 90Sr to the Barents Sea are similar to those for 137Cs, i.e. mainly global fallout, western European Reprocessing plants and fallout from the Chernobyl accident. A decline in activity concentrations in the water column might therefore be expected, as 90Sr is lost through radioactive decay (90Sr has a t of 28.5 years) and removal processes (biological uptake, adsorption to particulate matter followed by sedimentation of particulates etc.) 3.2.1.5 Plutonium in seawater Activity concentrations of 239,240Pu in the surface waters of the Barents Sea are shown in Figure 3.3. Levels vary in the range 6.6 9.9 mBq m -3. These activity concentrations compare with a mean levels (based on 15 measurements) determined in surface waters in 1995 (Grttheim, 1999) of 7.1 1.7 mBq m-3. The activity concentrations have fallen since the 1980s. Reported levels (Kershaw and Baxter, 1995) were in the range 17.1-18.0 mBq m -3 in 1981, 12.1-12.7 mBq m-3 in 1985 and 6.5 11.3 mBq m-3 in 1989. Evidence from 238 Pu:239,240Pu ratios suggested that these waters were a mixture of waters bearing both global fallout Pu and Sellafield-derived Pu at this time. In the early 1980s, global fallout was clearly the dominant source of Pu to the Barents Sea. However, a 238Pu:239,240Pu ratio of 0.11 (global fallout = 0.03-0.04; Sellafield = 0.2 based on cumulative Sellafield discharges) was observed in 1989 by Kershaw & Baxter(1995) and ratios mainly falling between 0.03 and 0.2, with some samples exhibiting ratios close to a pure Sellafield signal, were measured in the Barents Sea in 1995 (Herrmann et al., 1998; Grttheim, 1999) indicating a significant increase in the proportion of Pu isotopes in Barents Sea surface water that can be attributed to Sellafield releases. For the present study 238Pu:239,240Pu ratios in surface waters fall in the range 0.05-0.14 confirming the results from the studies in the mid 1990s. The presence of dissolved-phase Pu in the surface waters of the Barents Sea, at least at the time of sampling, appears to be derived predominately from global fallout with a smaller, though significant, component derived from Sellafield. The decline in surface seawater activity concentrations from the 1980s to the present (1999) might be attributable to a process involving the removal of Pu by biologically-mediated scavenging followed by downward transport and release back into solution at depth as described by Sholkovitz (1983). This leads to a subsurface maximum of dissolved Pu with

such profiles having been observed in open ocean environments receiving inputs from global fallout (Sholkovitz, 1983). Indeed data from 1995 (Herrmann et al., 1998; Grttheim, 1999) in many cases show distinct sub-surface maximum in activity versus depth profiles from the Barents Sea. In the present study, sub-surface water for Pu analyses was taken at only 2 stations. The results (Table 3.5) are not conducive to the formulation of robust conclusions and show that at Station 3 bottom water activities were higher than surface activities whereas at Station 6 bottom water activities were lower than surface activities. The bottom water taken at sampling station 3 is noteworthy by virtue of the fact that the associated 238Pu:239,240Pu is indicative of a pure Sellafield source.
Table 3.5 : 238Pu and 239,240Pu activity concentrations (mBq m-3) in suface and bottom sea water samples from Stations 3 and 6 in the Barents Sea. Station 3 (surface) 3 (bottom) 6 (surface) 6 (bottom) Depth (m) 0 132 0 230 Salinity 34.63 34.64 34.80 34.87
239.240

Pu (mBq m-3) 9.1 0.8 12.8 1.1 9.9 1.0 7.3 1.0

238

Pu (mBq m-3) 0.73 0.24 3.0 0.4 0.49 0.18 0.56 0.25

238

Pu:239.240Pu 0.08 0.03 0.23 0.04 0.05 0.02 0.07 0.02

Activity concentrations were fairly uniform over a large part of the sampling transect but fell slightly at locations very close to Kola Bay. The spatial pattern may reflect the fact that radionuclide inputs via the NCC do not dominate the inventory of 239,240Pu in the Barents Sea as they do for 99Tc and 137Cs. Pu isotopes derived from global fallout probably form a significant portion of the inventory associated with the Barents Sea and will of course have been introduced to the system in a uniform way.

Figure 3.3 : Levels of 239,240Pu (mBq m-3) in the surface waters of the Barents Sea - February 1999. Activity concentrations at each location are based on single measurements. Uncertainties (1 standard deviation) are in the range 8-18 %. Italicised figures in boxes represent 238Pu:239,240Pu ratios with uncertainties; n.d. = not determined owing to poorly-defined 238Pu activity concentrations.

3.2.1.6 Ultrafiltration of

239,240

Pu

Results from the ultrafiltration experiment on seawater samples are presented in Table 3.6. In all samples, the 239,240Pu activity concentrations in seawater filtered through a 0.45 m are higher than those filtered through a 10 kDa membrane. The colloidal fraction, in the size range 10 kDa < x < 0.45 m, of 239,240Pu varied between 10 and 25 %. Colloidal fractions of 239,240 Pu of the same magnitude have been reported for samples taken in the Lomonosov Ridge and Laptev Sea in 1996 (Mitchell et al., 1999). The colloidal material was believed to have a riverine provenance and was believed to play a potentially important role in the transport of particle-reactive contaminants from shelf areas to the Arctic interior. The provenance of the colloidal material in the present study cannot be clearly assigned. Large river systems discharging material into the Barents Sea are not present on the Kola Peninsular and it seems unlikely that the aggregate effect in terms of water and particulate matter discharges of regional rivers, e.g. Northern Dvina and rivers flowing into Murmansk fjord, could be on the scale as that observed for the great Siberian river systems, i.e. Ob, Yenisey, Lena, further east. Other mechanisms, for example in situ biogenically-mediated production of colloidal materials, should be considered in this case.

Table 3.6 : 239,240Pu activity concentrations in sea water following filtration by (i) 0.45 m filter and (ii) a 10 kDa filter.
239,240 Filter Pu (mBq m-3) 9.1 0.8 0.45 m 7.0 0.6 10 kDa 3 132 12.8 1.1 0.45 m 9.6 0.7 10 kDa 6 0 9.9 1.0 0.45 m 8.5 0.7 10 kDa 6 230 7.3 0.5 0.45 m 6.6 1.0 10 kDa * In this case defined as the size fraction 10 kDa < x < 0.45 m

Station 3

Depth (m) 0

% colloidal* 23 3 25 3 14 2 10 2

3.2.2 Radionuclides in sediment

The activity concentrations for 137Cs, 90Sr and isotopes of Pu are presented in Table 3.7. Levels are generally low in all cases and are comparable with regional activity levels reported in earlier work. For example, 137Cs and 239,240Pu activity concentrations measured in surface sediment (0-2 cm) in the summer of 1995 were 3.0-6.2 Bq kg-1 d.w. and 0.4-1.9 Bq kg-1 d.w. respectively as reported by Grttheim (1999). Activity concentrations in surface sediments (01 cm) from the open Kara Sea in the early 1990s were reported to range from 17-32 Bq kg -1 d.w. 137Cs and 0.4-1.3 Bq kg-1 d.w. 239,240Pu. The data that exist for 90Sr, as discussed in Section 3.1, show activity concentrations of 90Sr 0.32 0.15 Bq kg-1 d.w..

Table 3.7 : Activity concentrations of 137Cs, 239,240Pu and 90Sr in sediments of the Barents Sea.
Sr-90 Station No. Increment 3 3 3 3 3 3 3 6 6 6 6 6 6 6 6 0-2cm 2-4cm 4-6cm 6-8cm 8-10cm 10-12cm 12-14cm 0-2cm 2-4cm 4-6cm 6-8cm 8-10cm 10-12cm 12-14cm 14-16cm Bq/kg d.w. 0.61 0.32 0.49 0.72 0.52 na na 0.86 0.67 0.85 0.55 0.39 na na na 0.06 0.03 0.05 0.07 0.05 na na 0.09 0.07 0.09 0.06 0.04 na na na Bq/kg d.w. 4.7 3.7 3.3 2.8 3.2 6.1 2.4 5.7 7.4 4.2 12.6 5.3 3.5 3.2 5.3 Cs-137 Bq/kg d.w. 4.1 3.2 2 2.2 2.4 1.8 1.9 2.3 1 0.8 0.8 0.4 0.5 0.3 0.5 0.4 0.3 0.3 0.3 0.6 0.2 0.6 0.7 0.4 1.3 0.5 0.4 0.3 0.4 Bq/kg d.w. 0.42 0.41 1.52 0.2 <0.1 <0.09 <0.1 0.71 0.32 <0.1 <0.1 <0.1 <0.1 <0.09 <0.1 0.08 0.21 0.01 0.04 Bq/kg d.w. <0.35 0.37 <0.34 <0.35 <0.37 <0.33 <0.35 <0.35 <0.38 <0.39 <0.38 <0.35 <0.39 <0.35 <0.37 Std. dev Cs-137 Std. dev. Pu-239 Std. dev. Pu-240 Institute analyses AUN AUN AUN AUN AUN AUN AUN AUN AUN AUN AUN AUN AUN AUN AUN conducting

0.03 0.07

5 5 5 5 5 5 7 7 7 7 7 7 7 7

Std. dev Increment Sr-90 Bq/kg d.w. 0-1 cm 1.75 0.1 na 1-3cm na 3-5 cm 5-7 cm 7-9 cm 9-11 cm 0-2 cm 2-4 cm 4-6 cm 6-8 cm 8-10 cm 10-12 cm 12- 14 cm 14-16 cm 0.01 na 0.02 0.02 na na 0.01 na na na 0.01

Std. dev. Pu-239,240 Std. dev. 0.4 0.4 0.6 0.3 0.4 0.2 0.3 0.3 0.2 0.1 0.1 0.1 0.1 Bq/kg d.w. 1 0.69 0.5 0.17 0.25 0.1 0.52 0.35 0.08 0.037 0.024 0.006 0.022 0.035 0.1 0.05 0.04 0.02 0.02 0.01 0.07 0.03 0.01 0.008 0.006 0.007 0.007 IFE IFE IFE IFE IFE IFE IFE IFE IFE IFE IFE IFE IFE IFE

na = not analysed.

Sediment activity concentration data are further discussed under the investigative themes of Chapter 4.

3.2.3 Radionuclides in biota

Results from the analyses of biota samples are presented in Table 3.8.
Table 3.8 : Activity concentrations of 137Cs, 99Tc and 90Sr in biota from the Barents Sea.
Station Sample type
137

Cs w.w.

(Bq

kg-1)99Tc (Bq kg-1) d.w. 90Sr (Bq kg-1) w.w.

24 24 41 41 41 41 44 44 52 52 52 52 59 61 67 68 68

Cod (Gadus morhua) meat 70o16'N,37o24'E Cod (Gadus morhua) bone 70o16'N,37o24'E 72o36,4'N,38o58,7'E Shrimp (Pansereker) 72o36,4'N,38o58,7'E Seastar (Asteroidea)

0.0094 0.001 0.089 0.005 0.18 0.045 < 0.016 < 0.3 n.a. 0.0055 0.0005 < 0.3 < 0.3

Capelin (Mallotus villosus) meat, (n=30.14 0.045** 72o36,4'N,38o58,7'E for Cs-137) Polar cod (Boreogadus saida); (n=3 for0.14 0.02** 72o36,4'N,38o58,7'E Cs-137) 0.08 0.028 73o05,7'N,37o18,8'E Shrimp (Pandalus borealis) 73o05,7'N,37o18,8'E Shrimp (Pandalus borealis) - shell 0.08 0.022 71o34,6'N,36o15,5'E Shrimp (Pandalus borealis) 71o34,6'N,36o15,5'E Shrimp (Pandalus borealis) -shell Cod (Gadus morhua), meat; n=9 for Cs71o34,6'N,36o15,5'E 137) 0.27 0.11** 71o34,6'N,36o15,5'E Flounder (Pleuronectes flesus), meat 0.33 0.14** Plaice (Pleuronectes platessa), meat; 70o34,4'N,34o20,2'E (n=2 for Cs-137) 0.33 0.04** Haddock (Mellangrammus aeglefinus), 69o55,3'N,34o21,5'E meat (n=5 for Cs-137) 0.18 0.06** Norwegian haddock (Mellangrammusn.a 70o28,2'N,31o23,2'E aeglefinus ?) < 0.33 70o09,9'N,31o23,4'E Kamchatca crab : muscle < 0.25 70o09,9'N,31o23,4'E Kamchatca crab : roe

0.018 0.001* 0.045 0.003 0.032 0.002* 0.05 0.003 0.025 0.002 0.015 0.006 0.023 0.001 <0.007

< 0.3 0.015 0.001 < 0.3 n.a.

* meat only ** standard deviation if more than 1 sample analysed otherwise uncertainties = counting uncertainties.

Activity concentrations of 137Cs were at or below detection limits in many cases. Comparison with earlier data (as presented for the period 1991-1998 in Table 3.3.) suggests that activity concentrations in crustaceans (shrimp and Kamchatka crab) were lower in 1999 than the average levels for the preceding 7 years or so. This is however a tentative observation based on a very limited data set. The highest 137Cs activity concentrations were observed in demersal and benthic fish species namely Atlantic cod, plaice and flounder. The cod can be defined as second level predators feeding on capelin and polar cod. The data appear to indicate a bioaccumulation effect with higher concentrations of 137Cs at higher trophic levels although further data would be required to confirm this. Pronounced trophic level effects have been commonly observed in freshwater environments (Fleishman et al. (1994); Kryshev, 1995 Saxen & Koskelainen (1996). Plaice and flounder mainly feed on crustaceans and marine worms although larger individuals will prey on smaller fish species. The proximity of these fish to the sediment bed (which can be broadly defined as a sink for particle-reactive radionuclides) may increase the intake of radiocaesium through the ingestion of particulate matter during feeding. The physico-chemical form of 137Cs bound to sediments will influence the degree of uptake (through the gut) via this pathway. Activity concentrations of 99Tc were below detection levels in all cases. This was not a surprising result considering the low ambient seawater activity concentrations, especially in deep waters, and the low concentration factors for those species caught and analysed..

Organisms that are known to concentrate 99Tc to a high degree, such as Norwegian lobster, (Nephrops norvegicus) and lobster (Homarus gammarus) were not caught during trawling operations. Sr-90 activity concentrations were generally low. Maximum activity concentration of 0.045 0.003 Bq kg-1 w.w. and 0.089 0.005 Bq kg-1 w.w. were observed for shrimp shell and cod bone respectively. Strontium behaves as an analogue for Ca. Assimilation and incorporation into the exoskeleton (often formed from layers of chitin fibres intermeshed with proteins and, in many species, with calcium salts) of marine arthropods or the bone of fish (consisting of collagen and calcium, phosphate and carbonate minerals) is, therefore, expected. The activity concentrations for this study were similar to those reported in earlier studies (Table 3.3). Further analyses of these data have been conducted under Chapter 4.

3.3 Caesium-137 and technetium-99 in seaweed

Authors: Gordon C.Christensen, Elisabeth Strlberg: Institute for Energy Technology

Institute for Energy Technology has annually collected the brown alga Fucus vesiculosus at several sampling locations since 1980 (Figure 3.4), mainly in August and September (Christensen, 1986; Christensen and Selnaes, 1995). At the location Utsira, monthly samples have been collected regularly since January 1986, and at Tromya and Ingy since August 1998. Results from the locations 1 Grense Jakobselv, 3 Vard/Indre Kiberg, 4 Ingy and 6 Vestvgy will be presented here.
4. Ingy 3. Vard 2. Vads 5. Senja 1. Grense Jakobselv

6. Vestvgy

7. Vikna

8. Bud

9. Vgsy

10 A. Utsira

14. Hvaler 13. Tjme 12. Tromya 11. Lista

Figure 3.4 : Map showing IFE's sampling locations

3.3.1 Materials and methods

The Fucus samples were dried at 105 C, homogenised and analysed for gamma emitters using high purity germanium gamma spectrometry and computerised spectrum analysis. The 99 Tc-analyses at were performed at the University of Lund. The following analytical procedure was used: Technetium is extracted by TBP from sulphuric acid-hydrogen fluoride media. Backextraction is done from sodium hydroxide solution from which media technetium is electrodeposited onto stainless steel discs. As radiochemical yield determinant 99mTc is used. After decay of the yield determinant technetium is measured by an anticoincidence shielded GM counter (Holm et al., 1984).

3.3.2 Results and discussion

3.3.2.1 Caesium-137 The results for 137Cs in the Fucus samples from the four locations in northern Norway from August 1995 to August 2000 are shown in Figure 3.5. The four curves show very different shapes. The peak in the concentration in Fucus from Grense Jakobselv in 1998 is not found at the other three locations. The reason for this is not understood and will be studied closer.

1,2

1,0

0,8
Bq/kg d.w.

0,6

0,4

0,2

0,0 aug. 95

1 Gr. Jakobselv 3 Vard/I.Kiberg 4 Ingy 6 Vestvgy

aug. 96
137

aug. 97

aug. 98
Date

aug. 99

aug. 00

Figure 3.5 : Levels of samples)

Cs in Fucus at the four sampling locations (only August / September

The amount of radiocaesium originating from Sellafield in Fucus vesiculosus has steadily decreased since 1980. In the 1990s the highest concentrations of 137Cs have generally been

found in the Oslo Fjord and Skagerrak and decreases northwards. The Sellafield contribution at all these sites is now almost negligible. The term transit time has been used for the supposed maximum effect of a single discharge (Dahlgaard et al., 1997). Having estimated a representative transit time (t years), a Fucus transfer factor (FTF) can be calculated as the quotient between observed concentrations in the Fucus (Bq kg-1 d.w.) at the sampling site and an average discharge rate (PBq yr-1) t years earlier. The unit for the FTF then becomes Bq kg-1 d.w. / PBq yr-1. Calculations for IFEs southernmost locations have been performed earlier (Christensen & Strlberg, 2000). The results for Utsira are shown in Figure 3.6. A transit time of 4 years (Dahlgaard et al., 1997) from Sellafield to Utsira was used in the calculations. Based on these calculations, it is reasonable to suggest a transit time of 5 years to Vestvgy and 6-7 years to the three northernmost locations.
22,0 20,0 18,0 16,0 Bq/kg d.w. 14,0 12,0 10,0 8,0 6,0 4,0 2,0 0,0 80 82 84 86 88 90 Year 92 94 96 98 00
137

Measured Calculated Sellafield origin Calculated Baltic origin

Figure 3.6 : Calculated contributions from Sellafield and the Baltic Sea to the concentrations of in Fucus vesiculosus at the location Utsira

Cs

3.3.2.2 Technetium-99 The results for 99Tc in the Fucus samples from the four locations in Northern Norway from August 1995 to August 2000 are shown in Figure 3.7. The discharges of 99Tc from the EARP plant at Sellafield started late 1994. The discharge front seems to have reached all locations in the autumn of 1997. No sample was taken from Vard/Indre Kiberg in 1997, but it is reasonable to expect the same trend here as at Grense Jakobselv. An average transit time of 3-4 years has been calculated for 137Cs from Sellafield to Utsira (Dahlgaard et al., 1997). If the transit time for 99Tc is the same as for 137Cs, it would be reasonable to expect an average transit time for 99Tc from Sellafield to Vestvgy of 4-5 years and 5-6 years to the three northernmost locations. If this is the case, a decrease in 99Tc concentration should be expected in 2001.

A follow-up study of the monthly results from Utsira and Ingy will hopefully give information of actual transit times between Sellafield and the two locations and between the locations themselves.

400 350 300 Bq/kg d.w. 250 200 150 100 50 0 aug. 95 1 Gr. Jakobselv 3 Vard/I.Kiberg 4 Ingy 6 Vestvgy

aug. 96

aug. 97

aug. 98 Date

aug. 99

aug. 00

Figure 3.7 : Levels of 99Tc in Fucus at the four sampling locations (only August / September samples)

References
AMAP Assessment Report: Arctic Pollution Issues. Arctic Monitoring ana Assessment Programme. Oslo, 1998. BNFL (1995). Annual Report on Radioactive Discharges and Monitoring of the Environment 1994. British Nuclear Fuels plc., Directorate of Health, safety and Environmental protection, Risley, UK. Brown, J.E., Strand, P. & Bergan, T. (1999a). Modelling doses to biota in environmental systems // Extended abstracts of the 4th International Conference on Environmental Radioactivity in the Arctic. Edited by Per Strand and Torun Jolle. NRPA, Norway. P.125-128. Brown, J.E., Kostad, A.K.,Bringot, A.L.,Lina, B., Rudjord, A.L. & Strand, P. (1999b). Levels of 99Tc in biota and seawater samples from Norwegian coastal waters and adjacent sea. Marine Pollution Bulletin, 38 (7), pp. 560-571. Brown, J.E., Iospje, M., Kolstad, K.E., Lina, B., Rudjord, A.L. & Strana P. (in Press). Temporal trends for 99Tc in Norwegian coastal environments and spatial distribution in the Barents Sea. Journal of Environmental Radioactivity. Christensen, G.C., Radioactivity in Fucus vesiculosus along the Norwegian North Sea and Skagerrak coast 1980 - 1983, pp. 133-140 in "Study of radioactive materials in the Baltic Sea", IAEA-TECDOC-362 (1986). Christensen, G.C., Selnaes, T.D., Study of marine radioactivity along the Norwegian coast 1980-1994, pp. 618622 in Proceedings of an International Symposium on Environmental Impact of Radioactive Releases, IAEA, Vienna, Austria, 8-12 May 1995. Christensen, G.C., Strlberg, E., Can the outflow of radiocaesium from the Baltic Sea be detected in brown algae along the Norwegian coast? In Proceedings from the Marina-Balt Seminar, Stockholm, 9-11 June 1998, The radiological exposure of the population of the European Community to radioactivity in the Baltic Sea, Radiation Protection 110, EUR 19200, 433-438 (2000).

Chumichev, V.B. (1997). Long-term investigations of 90Sr content in the waters of the Arctic Ocean seas (White, Barents, Laptev, East-Siberian and Chukchi seas) // Extended abstracts of the Third International Conference on Environmental Radioactivity in the Arctic. Vol.2. Tromso, Norway. P.189-191. Dahlgaard, H., Bergan, T.D.S., Christensen, G.C., Technetium-99 and caesium-137 time series at the Norwegian coast monitored by the brown alga Fucus vesiculosus, in Proceedings Part 1 of International Symposium on Radionuclides in the Ocean RADOC 96-97, Cherbourg-Octeville, France, 7-11 October 1996, Radioprotection Colloques, Volume 32, C2 (1997) 353-358. Environmental Radioactivity in the Arctic and Antarctic (1993). Ed. by P.Strana ana E.Holm. sters, Norway. Environmental Radioactivity in the Arctic (1995). Ed. by P.Strand and A.Cooke. sters, Norway. Environmental Radioactivity in the Arctic (1997). Ed. by P.Strand. sters, Norway. Environmental Radioactivity in the Arctic (1999). Ed. by P.Strand and T.Jolle. sters, Norway. Fleishman, D.G., Nikiforov, V.A., Saulus, A.A. & Komov, V.T. (1994). 137Cs in fish of some lakes and rivers of the Bryansk Region and north-west Russia in 1990-1992. Journal of Environmental Radioactivity, 24, pp.145158. Grttheim, S. (1999). Artificial radionuclides in the Northern European Marine Environment in 1995. : Distribution of radiocaesium, plutonium, and americium in seawater and sediments. Cand. Scient thesis in Marine Chemistry. Department of Marine Zoology ana Marine Chemistry, Biological Institute, University of Oslo. Hermann, J., Levels of Man-Made Radioactivity in the Baltic Sea 1961-1995, Data Collected for the Marina Balt Project, Marina Balt Seminar, Stockholm, 9-11 June 1998. Nielsen, S.P., Radioactivity in the Baltic Sea: Modelling and Assessment of Doses to Man, Marina Balt Seminar, Stockholm, 9-11 June 1998. Holm, E., Rioseco, J., Christensen, G.C. (1983). 99Tc in focus from Norwegian waters. Proceeding sof the Symposium on the behaviour of long-lived radionuclides in the marine environment, La Spezia, Italy (1983), CEC, (revised version). Holm, E., Rioseco, J., Garcia-Leon, M., Determination of 99Tc in environmental samples, Nucl. Instr. Meth. Phys. Res., 223, 204 (1984). Holm, E. (1994). Polonium-210 and radiocesium in muscle tissue of fish from different Nordic marine areas. In: Nordic Radioecology. The Transfer of Radionuclides Through Nordic Ecosystems to Man. Ed. by H.Dahlgaard. Elsevier, 119-127. Kershaw, P. & Baxter, A. (1995). The transfer of reprocessing waste from north-west Europe to the Arctic. Deep sea Research II, 42 (6), pp.1413-1448. Kryshev, I.I. (1995). Radioactive contamination of aquatic ecosystems following the Chernobyl accident. Journal of Environmental Radioactivity, 27, pp.207-219. Leonard, K.S., McCubbin, D., Brown, J., Bonfield, R. & Brooks, T. (1997). Distribution of Technetium-99 in UK coastal waters. Marine Pollution Bulletin, 34, 628-636. Matishov, G.G., Matishov, D.G., Szczypa, J. & Rissanen, K. (1994). Radionuclides in the Ecosystem of the Barents and Kara Seas Region. Apatity, Kola Sci.Center Publ.House (in Russian). Mitchell, P.I., McMahon, C.A., Vinro, L.L. ana Ryan, R.W. (1998). Plutonium in Arctic surface and subsurface waters at the St Anna and Voronin Troughs. Radiation Protection Dosimetry. Vol.75, No.1-4, 247-252. Mitchell, P. et al. (1999). Radioecological assessment of the consequences of contamination of Arctic waters : Modelling the key processes controlling radionulcide behaviour unaer extreme conaitions (ARMARA). Contract no.,

F14P-CT95-0035. Final Report to the EC Nuclear Fission Safet Programme. Department of Physics, University College of Dublin. Nikitin, A.I. et al. (1994). Results of radionuclides analysis (waters, sediments ana biota). In: Radioactive contamination at dumping sites for nuclear waste in the Kara Sea. Results from Norwegian-Russian 1993 expedition to the Kara Sea. Osteras, NRPA. Nikitin, A.I., Bovkun, L.A., Katrich, I.Yu., Chumichev, V.B. ana Valetova, N.K. (1997). Field investigations of marine environment radioactive contamination in the seas of Eastern Russian Arctic during the year 1993 // Extended abstracts of the Third International Conference on Environmental Radioactivity in the Arctic. Vol.2. Troms, Norway. P.41-42. Radioactive Contamination in the Russian Arctic (1999). Report of Russian experts for AMAP. Saxen, R. & Koskelainen, U. (1996). Radioactivity of surface water ana freshwater fish in Finlana in 1991-1994. Finnish Centre for Radiation ana Nuclear Safety Report, STUK-A129. Strana, P., Rudjord, A.L., Salbi, B., Christensen, G., Foyn,L., Lina,B., Bjornstad, H., Bjerk, T., Nikitin, A.I., Kryshev, I.I., Chumichev, V.B., Dahlgaard, H. & Holm, E. (1993). Survey of artificial radionuclides in the Kara Sea. In: Environmental Radioactivity in the Arctic and Antarctic. Ed.by P.Strand and E.Holm. sters, 53-65. Strand, P.; Nikitin, A.I.; Rudjord, A.L.; Salbu, B.; Christensen, G; Foyn, L.; Kryshev, I.I.; Chumichev, V.B.; Dahlgaard, H. and Holm, E. (1994). Survey of Artificial Radionuclides in the Barents and the Kara sea//Journal of Environmental Radioactivity, Vol.25, No.1, p.99-112. Strand P., Nikitin A.I., Lina B., Salbu B., Christensen G.C., (1997). Dumping of radioactive waste and investigation of radioactive contamination in the Kara Sea. Results from 3 years of investigations (1992-1994) in the Kara Sea. Joint Norwegian-Russian Expert Group for investigation of radioactive contamination in the Northern Areas. sters: Norwegian Radiation Protection Authority, NRPA, 1997. Strand, P., Balonov, M., Aarkrog, A., Bewers, M.J., Howard, B., Salo, A & Tsaturov, Y.S. (1998). Chapter 8 : Radioactivity. In : AMAP Assessment Report : Arctic Pollution Issues. Arctic Monitoring and assessment Programme (AMAP), Oslo, Norway, pp. 525-620. Vakulovsky, S.M., Nikitin, A.I., Chumichev, V.B., & Malyshev, S.V. (1993). Radioactive contamination of the Barents ana Kara Seas. In: International Meeting on Assessment of Actual and Potential Consequences of Dumping of Radioactive Waste into Arctic Seas. Working Material. Oslo, February 1-5, 1993. Vienna, IAEA.

4. Mobility and uptake of radionuclides in marine systems

Authors : Peer Brretzen, Ole Christian Lind, Brit Salbu Agricultural University of Norway

4.1 Introduction
4.1.1 Mobility and bioavailability of radionuclides
The mobility of trace metals and radionuclides in the marine environment, their uptake in marine organisms and their toxicity are related to the physico-chemical forms i.e., their speciation. In natural waters, most radionuclides are present in different physico-chemical forms varying from low molecular mass (LMM) ions or molecules, via hydrolysis products and polymers to colloids and pseudo-colloids, or incorporated in inorganic or organic particles. The borderline between categories is difficult to establish and transformation among categories occurs gradually (Salbu, 1985). As natural waters are dynamic systems, the distribution of species exhibits spatial and temporal variations due to ongoing transformation processes. Sorption to available surfaces, complexation with available inorganic as well as organic naturally occurring ligands, polymerisation and aggregation of colloids, can transform LMM species into high molecular mass (HMM) species, whilst desorption, dissolution, displacement and dispersion processes may mobilise LMM species from solid surfaces. Thus, sediments can act as a sink for radionuclides for instance in effluents from nuclear installations or released from dumped waste. However, contaminated sediments may also act as a potential source of radionuclides to the water phase due to remobilisation of metals as dissolved species and resuspension of particles. The distribution of radionuclides between sediments and water (i.e. the distribution coefficient Kd) depends on the radionuclide species in question, sediment surface composition and is a function of contact time with the sediments. Furthermore, Kd is a conditional constant, i.e. it is susceptible to physical and chemical changes such as pH, temperature, salinity, redox conditions and sediment:seawater ratio (e.g. Davis and Kent, 1990). If the kinetics of the interactions in sediments is slow, then the apparent Kd may not reflect equilibrium conditions. Unless equilibrium conditions are confirmed, information about the kinetics of these interactions could be more relevant for predictive models than the apparent distribution of radionuclides between water and sediment. The reversible and irreversible interactions of trace metals and radionuclides with sediment surfaces in sediment-seawater systems can be distinguished using operational methods such as sequential extractions. The extraction scheme applied here is modified (Oughton et al., 1997) from the scheme devised by Tessier et al. (1979). Furthermore, information on kinetics can be attained from dynamic tracer experiments performed in laboratories. Marine organisms can accumulate cationic radionuclides from seawater via their gills, and from ingested contaminated particles via their digestive system. A common approach to assess the bioavailability of a contaminant is to estimate the bioconcentration factor (BCF [lkg-1]). The BCF concept implies that the radionuclide concentration in the organism is in direct proportion with the radionuclide concentration in the surrounding seawater. For filter

feeding organisms, such as the blue mussel Mytilus edulis, a major proportion of total body burdens of most metals might be derived from retained and particulate materials (e.g. ingested phytoplankton), and metal concentrations in Mytilus edulis do not always correlate with concentrations in solution or in macroalgae. However, for non-filter feeding organisms radionuclides are predominantly taken up in dissolved form via the gills, and it can be assumed that the uptake is related to ambient seawater concentrations of the radionuclides. In the present work model experiments using chemically well defined tracers have been applied to estimate the sediment-water interactions (Kd) and to estimate the retention of contaminated sediments in filter feeders (Brretzen, 2001).

4.2 Materials and methods

4.2.1 Mobility of radionuclides
The behaviour of Pu in the sediment-water system depends on the speciation (Tab. 4.1). The retention of mobile Pu-species in sediments may be negligible while corrosion particles and aggregating colloids containing Pu may settle. Furthermore, the interaction of Pu-species with sediments is a time and temperature dependant process. Under stable physical-chemical conditions (pH, redox, ionic strength) the distribution coefficient increases with time until pseudo-equilibrium/equilibrium is reached. Hence, the contact time between contaminated seawater and sediments should be taken into account in dispersion, ecosystem transfer and dose assessment models.
Table 4.1: Oxidation states of Pu in marine and natural waters (Skipperud et al., 2000).

OX.STATE Pu(III) Pu(IV) Pu(V) Pu(VI)

ION Pu3+ Pu4+ PuO2+ PuO22+

STABILITY Unlikely to exist in oxic waters, but may be present in anoxic waters and sediments. Easily oxidized to Pu4+. Hydrolysed Pu(IV) sorbs on colloidal and suspended material. Formation of Pu(OH)4 (am) in marine and natural waters. Most stable oxidation state in marine and natural oxic waters. Easily reduced to PuO2+.

In addition to measuring field samples (i.e. total concentrations), laboratory experiments have been performed to assess the interaction of Pu to operationally defined sediment fractions over time. These laboratory experiments have studied the interaction of Pu (V,VI)-species in the "Barents Sea sediment artificial seawater system" to obtain information of the timedependent distribution coefficient (Kd). The sediment samples used in the mobility experiments were collected from the Barents Sea (station 3). After a defined contact time, the samples have been sequentially extracted in order to determine easily mobilised and strongly associated fractions. Results from the laboratory studies were compared to field observations of Pu Kds and sequential extraction of environmentally contaminated sediments. Sorption experiment The tracer solutions were made from a stock solution of 400 Bq/l 236Pu(V,VI) in 1 M HNO3 (Chemical division of Harwell Laboratory, UK) and was diluted with artificial seawater and adjusted with 1 M NaOH to pH 5.9 prior to experiments. Aliquots of surface sediments (0-2 cm, 0.5 g d. w.) were transferred to centrifugation tubes, weighed and mixed with 18 ml artificial seawater. The samples were then conditioned for 2 weeks at 4C under oxic

conditions in the dark. 2 ml spiked artificial seawater was carefully added. The resulting pH of the solutions was 7.6. As a function of contact time, centrifugation tubes 1 day (n = 1), 1 week (n = 1) and 7 weeks (n = 3) were with-drawn, and the aqueous phase were removed after high speed centrifugation (Compact centrifuge, Avanti 30, Beckman) before determination of 236Pu. The temperature during experiment was 4C, and samples were stored under oxic conditions in the dark. The control tubes containing only seawater and tracer, show that sorption to tube walls was of minor importance (less than 5% absorption). Determination of Kd The ratio of radionuclides sorbed to sediment particles and dissolved in water at equilibrium when expressed as the distribution coefficient (Kd [ml/g]) is defined as:
Kd = Cs Cw

(4.1)

where Cs and Cw are the concentration of radionuclides in the sediment (Bq/g) and the seawater (Bq/ml) at equilibrium, respectively. The Kd values were calculated using sitespecific water concentrations, either from samples taken of surface waters or bottom water when applicable. To estimate the equilibrium value of Kd for Pu(V,VI) the Kd(t)-curve was fitted by,
K d (t ) = Kd (eq) ( 1 e t )

(4.2)

where Kd(eq) is the asymptotic value for Kd(t) reached at steady state, i.e. as t . Extraction studies Immediately after the withdrawal of seawater, the sediment samples were extracted sequentially using an established method (Oughton et al., 1992). The extractants and conditions used were: sea water, 1h at room temperature (RT); NH4Ac, sediment pH, 2 h RT; NH4Ac, pH 5, 2 h RT; NH2OHHCl, 6 h 80C; H2O2 + NH4Ac, 6 h, 80C; and 7M HNO3, 6 h, 80C. All extractions were carried out by shaking the samples with 20 ml of each extractant. The supernatant was separated from the solid by high-speed centrifugation. The solid phases were washed (10 ml of distilled water) and centrifuged between each extraction step. 236Pu concentrations in all samples were determined using low-level liquid scintillation. Plutonium determination 236 Pu was determined by means of low-level liquid scintillation (LKB Wallac, 1220 Quantulus). The aqueous phase of the samples was heated to dryness, partly digested by concentrated HNO3, taken up in 1 M HCl, added 50 mg ascorbic acid and mixed with Ultima Gold scintillation cocktail (Skipperud et al., 2000) The mix was counted using the beta-alpha discriminator (Yu-Fu, 1990). Extracts of the sediment without tracer were used as background, and to check for matrix effects. Detection limits ranged from 60 to 300 mBq/g sediment.

4.2.2 Biotest experiments with Mytilus edulis Sediment collection and characterisation
The sediment used in the biotest experiments was collected in the Stepovogo fjord at Novaya Zemlya (JRNC 1997) and stored in contact with circulating seawater prior to the experiment (Brretzen & Salbu, 2000). To characterise the sediment, grain size distribution, surface area, total organic carbon (TOC) and cation exchange capacity (CEC) analyses were performed using standard techniques. Macro and trace element concentrations were determined using Instrumental Neutron Activation Analysis (INAA). The sediment was wet sieved (mesh size 20 m) and only the < 20 m fraction was used in the exposure experiments with spiked suspended sediments.

Organism collection and handling

Mytilus edulis were collected from the Oslo Fjord. The blue mussels collected were scraped clean of epibiota and weighed. About 150 mussels weighing between 17 - 23 g (wet weight) were selected and placed in 4.7 l polypropylene cages (Nalgene) in two large flow-through tanks (92 58 22 cm; 115 l). Seawater (26 salinity) was directly pumped into the tanks from the Oslo fjord at a rate of about 1 l/min from 1 m depth. In addition, the water was circulated by a submerged water pump (Maxi jet MJ 500, Agna systems, Italy) with a water circulation rate of 500 l/h to assure flowing aerated water around the filtering mussels. The mussels were acclimated for 1 week prior to the experiments. Tracers used and spiking of sediments Cationic tracers added to hollow-fibre filtered (< 10 kDa; Amicon, Inc. USA) seawater were used for dissolved tracer exposure experiments. The gammatracers used were 134Cs (t1/2 2.1 years, 605 and 795 keV) and 60Co (t1/2 5.27 years, 1173 and 1333 keV) with a decay corrected specific activity of 166 and 4050 MBq/mg, respectively (Nycomed-Amersham PLC., UK). The particle exposure experiments were undertaken using the < 20 m sediment fraction. The < 20 m sediment fraction was equilibrated with seawater for 4 weeks before cationic tracers were added to the slurry and allowed to interact for 4 months, to allow the tracers to associate strongly with the sediment particles. Before exposure, the spiked sediment particles were washed with seawater several times until the amount of tracers in the seawater wash became negligible.

Uptake experiments from tracers in ultrafiltered seawater

By using ultrafiltered seawater (< 10 kDa), interactions between the gammatracers and particles usually present in seawater (e.g. phytoplankton) are avoided and the organisms are therefore exposed to LMM species only. In the uptake experiments of LMM species to the organisms, a kinetic approach has been used. As depuration of contaminants from the organism and the growth rate (Wang et al., 1996) in short term uptake experiments can be assumed to be negligible, the concentration of contaminants taken up by the organism is a function of the water concentration only. Consequently, the short-term uptake of dissolved tracers can be expressed by: dCo = r01 Cw dt where r01 is the LMM uptake rate coefficient on a dry weight basis [mlgd.w.-1h-1]. (4.3)

To study the uptake of LMM tracers in Mytilus edulis the organisms were placed in tanks filled with ultrafiltered (< 10 kDa) seawater. After an acclimation period (15 minutes) the seawater was spiked with the gammatracers 134Cs and 60Co. During the uptake experiment (2 hours), individually numbered organisms were whole body counted for gamma activity at different time intervals. Furthermore, additional mussels were withdrawn after different exposure during the uptake period and soft tissues were separated from the shell and counted separately. Prior to the whole body counting, all organisms were rinsed with clean seawater, and counting times were 2-5 minutes. After the uptake period, the whole body monitored and the remaining organisms were transferred to large flow-through tanks for depuration monitoring.

Uptake experiments of tracers associated with suspended sediments

To measure the uptake of metals from spiked sediments via ingestion, mussels were placed in separate tanks with ultrafiltered (< 10 kDa) seawater containing sediments (< 20 m) spiked with Cs and Co tracers. Before added to the exposure tanks, the tracers had been in contact with the sediments for 4 months and the sediment had been repeatedly washed with seawater several times to remove any desorbed tracer. These experiments had a pulse-chase design as described by Decho & Luoma (1991), with a spiked sediment hot feed period of 25 minutes. After this hot feed period, individually numbered organisms were rinsed with clean seawater and whole body counted to determine the total amount of ingested spiked sediments. After the hot feed period, the mussels exposed to spiked sediments were transferred to a large flow-through tank for depuration monitoring. It is difficult to measure the uptake rate coefficient for particle associated radionuclides (r 01,s [mggd.w.-1h-1]) directly from sediment uptake experiments. However, r01,s can be estimated indirectly by using the following expression (Landrum et al., 1992): r01,s = AEIR (4.4)

where AE is the assimilation efficiency of the tracer associated with the sediment phase [unit less] and IR (ingestion rate) is the flux of sediments through the digestive system [mggd.w.-1h1 ]. The AE is the fraction of tracer that is retained (assimilated) in the organism after a pulse of contaminated sediments has passed through the organism. There are two advantages obtained by exposing the mussels to sediments labelled with radioactive tracers for a short time period (20-30 min), and thereafter transferring them to uncontaminated environments. Firstly, desorption of tracer from the sediments to the water phase is minimised, and therefore the mussels are predominantly exposed to tracers via sediment ingestion. Secondly, by following a pulse of labelled sediments through the digestive system of the organisms the AE is easily obtained, as the intercept of the slow component with the y-axis. The IR was not determined in this experiment but estimations of the IR can be found elsewhere, e.g. Hawkins et al. (1998).

Depuration experiments
After the organisms are transferred to clean environments (Cw = 0) and uptake of contaminants no longer occurs, the depuration can be followed. As an initial rapid and a subsequent slower elimination rate can describe the depuration curve, the total concentration of the gammatracer within the organism during depuration can be expressed as:

Co = C1e k1t + C2e k2 t

(4.5)

where C1 and C2 are the intercepts of the lines having slopes k1 and k2, respectively, and Co = C1 + C2 at the start of the depuration experiment. The four parameters are readily found by non-linear regression. The initial phase of depuration represents elimination from the central compartment (Fig. 4.5), while the later phase represents redistribution from the second, peripheral compartment (Fig. 4.5) within the animal (Spacie & Hamelink, 1982).

Water

r01

r10 Organism central compartment

r12 r21

Organism peripheral compartme nt

Figure 4.5: A model of the water-organism system, where the organism is divided into two compartments (Brretzen, 2001).

The depuration of tracers from the contaminated mussels was followed in the large flowthrough tanks for about 1 month. Uncontaminated organisms also kept in the depuration tanks were routinely measured to detect any cross-contamination. During the experiments the pH, temperature and dissolved O2 concentration were continuously logged and salinity was measured daily using a multisensor logging to a computer. Whole body counting was performed at different time intervals on each of the individually monitored organisms during the depuration period. The bioconcentration factor (BCF [lkg-1]) is defined as: BCF = Co Cw (4.6)

where Co is the concentration of the contaminant in the organism on a wet weight or dry weight basis [gkg-1 or Bqkg-1], and Cw is the concentration of the contaminant in the surrounding water [gl-1 or Bql-1] at steady state. By applying the BCF concept to marine organisms it is assumed that the metal concentration in the organisms is at steady state with the concentration in the surrounding water and that the uptake of the metal is in proportion to its concentration in the seawater (Luoma, 1983).

Tracer measurements
An automatic NaI-system (Packard, Minaxi Autogamma 5000) was used to determine the tracer activity in the seawater at different time intervals during the LMM exposure and in dissected mussel parts, while a NaI-detector with a multichannel analyser (S10 plus, Canberra) was used for whole body counting of mussels. The two detectors were intercalibrated and the results were corrected for the difference in counting geometries.

4.3 Results and discussion

4.3.1 Mobility of radionuclides - Results from Barents Sea field data
The activity concentration levels for 239Pu, 90Sr and 137Cs in the sediments are generally low and similar to earlier reported values from the same area (JRNC, 1997; Salbu et al., 1997). Figure 4.1 show that the activity concentration of 90Sr is quite constant down the 10 cm profile. For 239Pu there is a significant increase in the activity concentration at 4-6 cm depth, possibly due to heterogeneities such as radioactive particles in the sediment material. The activity concentration of 137Cs at station 3 in Fig. 4.1 shows a slow decrease with depth, except at 10-12 cm where the highest activity concentration were measured, also possibly due to radioactive particle heterogeneities.

Cs-137 0-2 cm 0-2 cm 2-4 cm Depth (cm) 2-4 cm 4-6 cm Depth (cm) 6-8 cm 8-10 cm 10-12 cm 8-10 cm 12- 14 cm 0 0.2 0.4 0.6 0.8 1 1.2 1.4 1.6 1.8 0 1 2 3 4 Bq/kg dry weight 5 6 7 8

4-6 cm

Pu-239 Sr-90

6-8 cm

Bq/kg dry weight

Figure 4.1 : Vertical distribution of 239Pu, 90Sr and 137Cs in sediment profiles collected at station 31.

The activity concentrations of 239Pu and 90Sr at station 6 are shown in Fig. 4.2. For both radionuclides a decrease of the activity concentration with depth is indicated. The activity concentration of 137Cs with depth at station 6 in Fig. 4.2 shows a somewhat irregular depth profile, possibly indicating heterogeneously distributed radioactive particles in the sediment core.

Cs-137

0-2 cm
0-2 cm

2-4 cm De pt h 4-6 cm (c m) 6-8 cm

2-4 cm 4-6 cm Depth (cm)

Pu-239 Sr-90

6-8 cm 8-10 cm 10-12 cm 12- 14 cm

8-10 cm

14-16 cm

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

0.9

6 Bq/kg dry weight

10

12

14

Bq/kg dry weight

Figure 4.2 : Vertical distribution of 239Pu, 90Sr and 137Cs in sediment profiles collected at station 61.
1

Error bars are based on average deviation from mean value (n=2) for 239Pu.

The calculated field Kd values (Table 4.2) for 90Sr are approximately a factor 2 2.5 lower, while the calculated 137Cs values are approximately a factor 1.5 2 lower than the IAEA recommended values, but the calculated Kds for both radionuclides are well within the range reported by IAEA. The Kd values are, however, in agreement with previous reported Kd values from the Barents and Kara Sea area (Salbu et al. 1997; Carroll et al., 1997; 1999; Fisher et al., 1999), and emphasizes the necessity of deriving site-specific data for radionuclide transport models. The 239+240Pu Kd values agrees well with the IAEA recommended value, and with previously reported field values from the region (Fisher et al., 1999).
Table 4.2 : Field derived distribution coefficients compared with Fisher (1999) and IAEA (1985) recommended Kd values.

Kd [l/kg] St 3 St 5 St 6 Fisher (1999) IAEA (1985)

Sr 370* 489* 100 (4-300) 1000 (100-5000)

Cs 1378 1306* 2280 1000 (100-20000) 3000 (100-20000)

Pu 3104 1.1105* 1.1105 1105 (8104-2105) 1105 (1104-1106)

*based on surface water activity

Kinetic tracer experiments The interaction of Pu-species with sediments follows a two step reaction (Fig. 4.3) as earlier shown by Skipperud et al. (2000). With time there is a reduction in the mobile fractions and an increase of the Pu activity concentration in more strongly bound sediment fractions (Fig. 4.4).

1000

Kd [ml/g]

Chi^2 = 12857 A 736.21 114.38 k 0.00622 0.00291

100

200

400

600

800

1000

1200

Contact time [hours]

Figure 4.3 : Laboratory derived Kd as a function of contact time for Pu(V,VI) in a Barents Sea sediment- artificial seawater system.

The calculated Kd(eq) value for Pu(V,VI) (740 ml/g) is low compared with field derived Kds in the current study and with results reported by IAEA (1985), but in agreement with

previously published laboratory derived Kd values for Pu(V,VI) (Skipperud et al., 2000). The variation is possibly due to differences in Pu-speciation (Pu(III,IV) has higher Kd), sediments characteristics and sediment-seawater ratio. The current Kd is derived from a system with a high sediment-seawater ratio (see chapter 2) and should be applicable to leakage of ionic Pu(V,VI) from dumped objects embedded in sediments.

H2O

NH4Ac pH = 7 F r a c NH4Ac pH = 5 t i o n NH2OH.HCl

1d 6d 47 d

Ox. fraction (H2O2 + HNO3) 0 10 20 30 %Extracted 40 50 60

Figure 4.4 : Sequential extractions of Barents Sea sediments contaminated with Pu (V,VI) and stored under oxic conditions at 4C. The oxidisable fraction (Ox. fraction) comprises the H2O2- and HNO3 fractions.

4.3.2 Bioavailability of radionuclides Activity levels in biota bioconcentration factors

Low concentrations of 137Cs (0.08-0.18 Bq/kgw.w.) and 90Sr (0.018-0.032 Bq/kgw.w. in muscle, and 0.045-0.05 Bq/kgw.w. in shell) were found in the shrimp Pandalus borealis, while 99Tc concentrations were under the detection limit of 0.3 Bq/kgd.w.. In starfish (Asteroidea sp.) and in muscle and roe from the Kamtchaka crab (Paralithodes camtschaticus), 137Cs and 99Tc activity levels were under the detection limit of 0.3 Bq/kgw.w.. In cod (Gadus morhua) the concentrations of 90Sr in muscle were 0.0094-0.025 Bq/kgw.w., while somewhat higher in bone 0.089 0.005 Bq/kgw.w., and similar low concentrations of 90 Sr were measured in muscle from the fish species Capelin (Mallotus villosus), Flounder (Pleuronectes flesus), Plaice (Pleuronectes platessa) and Haddock (Mellangrammus aeglefinus). The field derived BCFs presented in Table 4.3 were calculated for the different species using an average value of the measured seawater concentrations of the radionuclides i.e. 3.3, 0.68 and 1.7 Bq/m3 for 137Cs, 99Tc and 90Sr, respectively. The BCFs for 137Cs measured in shrimp agree very well with the IAEA (1985) recommended value for crustaceans, and are in good agreement with earlier reported BCF values for crustaceans from the Kara and Barents Seas (Fisher et al., 1999). The BCFs for Tc are at least a factor 2 lower, and the Sr values are a factor more than 5 higher for shrimp than the IAEA recommended values. The BCF values for Sr in fish are, however, in agreement with the IAEA values, and with previous reported values from the region (Fisher et al., 1999).
Table 4.3 Field derived bioconcentration factors (BCF) compared with IAEA (1985) recommended BCF values.

BCF (l/kgw.w.) Shrimp Crustaceans - IAEA* Fish Fish - IAEA*

Cs 24-54 30 (10-50) -

Tc < 444 1000 (500-50000) -

Sr (muscle) 11-19 2 (0.1-5) 6-15 2 (0.3-10)

Sr 26 (shell) 52 (bone)

*IAEA (1985) recommended values (based on soft parts)

Laboratory experiments - Uptake and depuration from ultrafiltered seawater

By using ultrafiltered seawater (< 10 kDa), interactions between gammatracers and particles usually present in seawater (e.g. phytoplankton) are avoided and the mussels are exposed to LMM species only. The uptake of LMM gammatracers in whole mussels as well as in the soft parts and shell is shown in Figure 4.6.
Conc. in mussels [Bq/gd.w.]

Figure 4.6: Uptake of cationic 134Cs and 60Co tracers added to ultrafiltered seawater (< 10 kDa) in Mytilus edulis (n = 4, error bars 1 sd). For each tracer the uptake rate is estimated by linear regression (with the error bars as weights) for soft parts, shell and whole mussel. The concentration is plotted as a function of the exposure, i.e. the time integrated tracer concentration in the water. The 95 % confidence intervals are given as dotted lines (Brretzen, 2001).
5 5 5 0
14 3

C s

10 1 10 0

6 0

C o

Concentration in mussels [Bqg ]

4 5 4 0 3 5 3 0 2 5 2 0 1 5 1 0

9 0 8 0 7 0 6 0 5 0 4 0 3 0 2 0 1 0

Sf p rs ot at Se h ll W l ms e h e us l o

The concentration of the tracers in mussels [Bqkgd.w. ] is plotted as a function of the exposure, i.e. time integrated radionuclide concentration in the seawater. The data was fitted using linear regression with the standard deviations as weighing factors, and the gradient of the regression curve gives the uptake rate coefficient (r01). For each radionuclide, the regression lines (for soft parts [Bqgd.w.(soft parts)-1], shell [Bqgd.w.(shell)-1] and whole mussel [Bqgd.w.(soft parts+shell)-1]) are drawn (Fig. 4.6) with 95 % confidence intervals (plotted lines), and r01 for soft parts are presented in Table 4.4. The high uptake rate for soft parts compared to shell and whole mussel are mainly due to the low dry weight of the soft parts relative to the shell.
d.w. -1

-1

5 0

1 0

1 5

2 0

2 5

3 0

1 0

1 5

2 0

10 2 10 1 10 0

19 0

C d

9 0 8 0 7 0 6 0 5 0 4 0 3 0 2 0 1 0

6 5

Z n

9 0 8 0 7 0 6 0 5 0 4 0 3 0 2 0 1 0

1 0

1 5

2 0

2 5

3 0

3 5

0 -, 0 5

0 , 0

0 , 5

1 , 0

1 , 5

2 , 0

25 ,

3 , 0

3 , 5

4 , 0

Ep s r [ q / l] x o ue B m h

Exposure [Bq h/ml]

Table 4.4: Laboratory derived rate constants (Fig. 4.5) and BCFs for mussel soft parts (dry weight) when exposed to cationic tracers added to ultrafiltered seawater (Brretzen, 2001).

soft parts
134

Cs

60

Co

r01 [mlgd.w.(soft)-1h-1] 1.1 0.1 1.9 0.4

r10 [h-1] 0.015 0.007 0.00035 0.00023

r12 [h-1] 0.042 0.009 0.031 0.021

r21 [h-1] 0.014 0.002 0.041 0.011

BCF 300 140 9 700 6 600

The depuration curves, i.e. tracer concentrations in whole mussels after transfer to clean seawater are shown in Figure 4.7. The depuration followed a multi-exponential release, and the whole body depuration curves were best described with a model having three exponential 2 functions, when comparing the values for models with two and three exponential functions.

The dissected mussels were divided into soft parts and shell, and the depuration curves were fitted for each part using non-linear regression (Fig. 4.8). The depuration of the two parts was best described with a model containing two exponential functions when using the same criteria as for whole mussel data. The fast and the slow compartment in the soft parts can be attributed to egestion and physiological turnover, respectively. The two compartments in the shell depuration model indicate that there are at least two different types of binding sites available on the shell surface.
Figure 4.7: Depuration from Mytilus edulis after 2 hours uptake of cationic tracers added to ultrafiltered seawater (< 10 kDa) using in vivo gamma spectrometry (n = 4, error bars 1 sd). The data are best fitted with a non-linear regression model having three exponential functions (Brretzen, 2001).
Fraction retained
1
14 3

Cw e s ar t

6 0

C we o ar t

Fraction retained

0 , 1

0 , 1

M e E D a3 o l x e y d: p c

M e E D a3 o l x e y d: p c 01 . 9 0 01 . 2 1 01 . 5 0 3 . 0 01 . 0 0

0 01 = . 04 0 C1 = . 8 0 0 6
2

0 04 = . 06 0 C1 = . 1 0 2 3
2

02 . 7 0 05 . 6 1 03 . 0 0 2. 1 8 03 . 0 0 20 0

k1 = . 2 0 3 2 C2 = . 6 0 9 1 k2 = 3 1. 7 C3 = . 5 0 2 1 k3
1 1

k1 = . 9 0 3 4 C2 = . 6 0 3 1 k2 = 5 5. 6 C3 = . 2 0 5 5 k3
1 1

The rate constants (r10, r12, r21) and BCFs were calculated on a dry weight basis from the regression parameters and are presented in Table 4.4. Table 4.4 shows that the laboratory derived BCF for the monovalent alkali metal Cs (class A) is at least a factor 20 lower than for the divalent cation Co (borderline class). The uptake rate coefficients (Tab. 4.4) show that the uptake rate in mussels is higher for Co than for Cs, while the depuration rate is highest for Cs and lowest for Co. The low BCF for Cs can therefore be explained by a low uptake rate and a very high depuration rate.
=9 40 7 0 = 30 14

01 , 0

01 , 0

20 0

40 0

60 0

80 0

10 00

20 0

40 0

60 0

80 0

10 00

19 0

Cwe d ar t

6 5

Z we n ar t

0 , 1

0 , 1

M e E D a3 o l x e y d: p c

M e E D a3 o l x e y d: p c

0 04 = . 06 0
C1 = . 9 0 9 2
1

0 03 =. 1 0
C1 = . 9 0 0 3
1

03 . 2 0

09 . 1 0

k1 = . 3 0 6 4 C2 = . 9 0 2 2 k2 = 3 2. 6 C3 = . 0 0 9 4 k3
1 1

07 . 1 3 02 . 4 0

k1 = . 8 1 0 C2 = . 7 0 7 4 k2 = 3 1. 7 C3 = . 4 0 3 1 k3
1 1

05 . 4 08 . 3 0 3 . 9 02 . 0 0 56 48

4 . 7 01 . 4 0 82 3

= 26 33

= 50 30

01 , 0

01 , 0

20 0

40 0

60 0

80 0

10 00

20 0

40 0

60 0

80 0

10 00

D u to tm[ r ] e r i ni eh pa s

To compare the laboratory derived BCFs with time [hrs] Depuration data published by IAEA (1985), the BCFs were recalculated on a wet weight basis. For Cs in soft tissues the wet weight BCF (34) agrees well with the IAEA recommended value of 30 and field derived values for molluscs in the Kara and Barents Sea (Fisher et al. 1999). The wet weight BCFs for Co (1 100) are lower than the IAEA recommended values, but within reported ranges (BCF range for Co: 1103 1105). The somewhat low BCFs calculated in this work can be primarily explained by low uptake rates. For Co, the uptake rates were about 70 % lower than in experiments performed by Wang et al. (1996), indicating that the mussels in this experiment were filtering water at a lower rate. Both physiological and experimental factors may be of importance explaining these differences. Long acclimation periods may reduce stress effects, but this is countered by Dahlgaard (1981) and Widdows & Hawkins (1989) who observed that mussels might filter lower quantities of water when placed in water where algal cells are absent for longer periods (> 2 hours). A relatively short acclimation period (15 minutes) was therefore chosen for these experiments.
Figure 4.8: Depuration from soft parts () and shell () after 2 hours uptake of cationic tracers added to ultrafiltered seawater (< 10 kDa) using data from dissected mussels (n = 3, error bars 1 sd). The data are best fitted with a non-linear regression model having two exponential functions (Brretzen, 2001).
14 3

Fraction retained

C ar s t w e
1
Sl hl e M l E Da o : x ey d e p c2

6 0

1
Stpt o a f r s M l EDa o : x ey d e p c2

Cw r oa t e

. 0 8 =01 0 0
C1 =. 3 0 1 7 k1 =4 17 . C2 =. 4 0 1 1
1

. 7 =8E 4 76
02 . 5 0 1 . 3 02 . 5 0 1 2 7 C1 =. 8 0 4 1 k1 =. 4 9 2 C2 =. 1 0 4 0 k2
1 1

00 . 3 0 03 . 4 00 . 2 0 2 5 8

0 , 1

k2

=2 3 6

=3 5 8

0 , 1

Fraction retained

Stpt o a f r s M l EDa o : x ey d e pc2

Sl hl e M l EDa o : x ey d e p c2

. 0 5 = 00 0 0
C1 =. 0 0 8 1 01 . 0 0 3 . 5 00 . 7 0 21 7 6

. 0 1 =0 6 0 3
C1 =. 2 0 7 4 k1 =0 12 . C2 =. 6 0 7 3 k2
1 1

08 . 4 0 5 . 4 05 . 4 0 6 0 0

01 , 0

01 , 0

k1 =4 10 . C2 =. 4 0 3 1 k2
1

=9 48 9

=0 19 7

1E 3 0 1 0 0 2 0 0 3 0 0 4 0 0 5 0 0 6 0 0 7 0 0 8 0 0

1E 3 0 1 0 0 2 0 0 3 0 0 4 0 0 5 0 0 6 0 0 7 0 0 8 0 0

19 0

C ar d t we

6 5

Zw r na t e

0 , 1

0 , 1

01 , 0

Stpt o a f r s M l EDa o : x ey d e p c2

Sl hl e M l EDa o : x ey d e p c2

01 , 0
01 . 3 0 05 . 3 00 . 7 0 6 8

Stp t o a f r s M l E Da o : x ey d e pc2

Sl hl e M l EDa o : x ey d e p c2

. 0 9 =0 3 0 0
C1 =. 7 0 8 0 k1 =1 19 . C2 =. 2 0 9 5 k2
1 1

. 0 5 =0 0 0 0
02 . 7 0 13 3 . 02 . 2 0 23 1 1 C1 =. 9 0 1 3 k1 =. 7 4 4 C2 =. 9 0 2 0 k2
1 1

. 0 3 = 00 0 0
C1 =. 9 0 4 2 k1 =. 8 7 2 C2 =. 8 0 4 1 k2
1 1

. 0 9 = 00 0 0
00 . 8 0 01 . 5 00 . 4 0 1 3 6 C1 =. 1 0 4 5 k1 =. 7 5 6 C2 =. 2 0 9 1 k2
1 1

01 . 6 0 04 . 4 01 . 0 0 5 9

=8 41 8

=4 3 3

=3 17 6

=8 2 8

1E 3 0 1 0 0 2 0 0 3 0 0 4 0 0 5 0 0 6 0 0 7 0 0 8 0 0

1E 3 0 1 0 0 2 0 0 3 0 0 4 0 0 5 0 0 6 0 0 7 0 0 8 0 0

D u to tmh ] e r i ni e r pa [ s

Depuration time [hrs]

Ingestion and depuration of metals associated with particles

The Stepovogo sediment sample is characterised by a high fraction of silt, and a low concentration of organic substances (Tab. 4.5). Grain size analysis of the < 20 m wet sieved sediment shows that the clay fraction is about 18 %.
Table 4.5: Loss on ignition (LOI), Total organic carbon (TOC), Sediment surface area (Sg), grain size distribution and stable element concentration in sediments (Brretzen, 2001).

LOI TOC
[%] [%]

Sg
[m2/g]

20 - 6 6 - 2
[m] [m]

<2
[m]

Cs

Co 28

[mg/kg] [mg/kg]

Fe
[g/kg]

0.97

13.3

37 % 45 % 18 % 7.3

52

The depuration curves after the short-term sediment ingestion period are shown in Figure 4.9. The data were fitted using non-linear regression. A depuration model having two exponential 2 functions was most appropriate (when comparing the values), in contrast to the threeexponential depuration model that was most appropriate when describing depuration after dissolved tracer uptake. The two depuration components may reflect fast egestion (with a half life of about 2.5 hours) of gammatracer associated to sediment particles and a slow physiological turnover of the tracer (half lives of about 250 1000 hours).

Fraction retained

Fraction retained

Figure 4.9: Depuration from Mytilus edulis after 25 minutes feeding with tracer-associated sediments (< 20 m) suspended in clean seawater using in vivo gamma spectrometry (n = 4, error bars 1 sd). The data are best fitted with a non-linear regression model having two exponential functions (Brretzen, 2001).
1
14 3

C s d et s ei n m

6 0

C s d et o e im n

M e Ep ea2 o l: x Dc y d

0 03 =. 3 0
2

C1 = . 6 0 6 9
1

0 5 . 9 0

k1 = . 6 3 0 C2 = . 0 7 0 8 1 k2
1

0 6 . 4 00 0 .3

=8 57

59 9

0 , 1

0 , 1

Md l Ep ea2 o e x Dc y :

0 08 = . 17 0 C1 = . 1 0 4 7
2

04 . 4 0 03 . 6 02 . 5 0 8 3

k1 = . 6 3 9 C2 = . 3 0 9 3
1 k2- = 7 31

01 , 0 0 20 0 40 0 60 0 80 0 10 00

01 , 0 0 20 0 40 0 60 0 80 0 10 00

The AEs and the rate constants are presented in Table 4.6. The depuration curves after sediment ingestion are similar to the depuration curves after uptake of dissolved tracers, with a fast depuration of Cs. The AE for Co (34 %) is the same as reported by Gagnon & Fisher (1997) for Co associated with silica particles coated with fulvic acid.
1 1
19 0

C s d et d e im n

6 5

Z s d et n e im n

0 , 1

0 , 1

Md l Ep ea 2 o e x Dc y :

Md l Ep ea2 o e x Dc y :

00 1 3 = . 01 C1 = . 2 0 0 8
2

03 . 3 0

0 09 = . 27 0 C1 = . 5 0 1 8
2

05 . 7 0

k1 = . 4 3 9 C2 = . 1 0 9 2

04 .3 01 . 7 0 54 2

k1 = . 3 2 3 C2 = . 9 0 8 1
1 k2- = 1 81

08 . 3 02 . 9 0

k2-1 = 4 8 11

40 1

01 , 0 0 20 0 40 0 60 0 80 0 10 00

01 , 0 0 20 0 40 0 60 0 80 0 10 00

Dp r t n im [ r ] e uaio t e hs

Table 4.6: AEs and rate constants for mussel soft parts (dry weight) when exposed to tracers Depuration time [hrs] associated with sediment particles. The rate constants are calculated from the regression coefficients estimated from the depuration experiments (Brretzen, 2001).

134

Cs

60

Co

AE [fraction] 0.11 0.03 0.34 0.03

r10,s [h-1] 0.016 0.008 0.0082 0.0201

r12,s [h-1] 0.28 0.05 0.16 0.36

r21,s [h-1] 0.035 0.005 0.083 0.112

4.4 Conclusions
The concentration of radionuclides in marine organisms in the Barents Sea is generally low, and seems (in most cases) to be in proportion with surrounding seawater concentrations. Generally the field based Kd values agree well with other previous studies from the area and emphasize the importance of site-specific data, as the present results are lower than the generic IAEA (1985) data. The laboratory based tracer experiments show that the sorption of Pu(V,VI) to sediments is a time dependent process, and several months are needed to reach semi-equilibrium. Kinetic tracer experiments are useful to estimate the BCFs, and the results are in agreement with field derived BCF ranges published in IAEA (1985) and Fisher et al. (1999). The uptake experiments of LMM radionuclides in Mytilus edulis showed that the uptake rate coefficients is higher for Co than for Cs, and the calculated BCFs increased accordingly. The depuration of the tracers in the mussels could be described by multi-exponential functions, and a twocompartment model was used to estimate the uptake and depuration kinetics of the contaminants within the mussels. Laboratory experiments were also well suited for estimating the AEs for the tracers studied, used to assess the retention of resuspended contaminated particles in mussels in a model based on toxicokinetic considerations (Brretzen, 2001). Furthermore the results show that resuspended contaminated sediments may represent an important pathway for radionuclides such as Co and Cs to the filter feeding Mytilus edulis.

References
Brretzen P (2001) Mobility of trace metals and radionuclides in sediments and bioavailability of resuspended sediments (Paper V). PhD Thesis. ISBN: 82-575-0447-5. 124p. Brretzen P, Salbu B. (2000) Estimation of apparent rate coefficients for radionuclides interacting with marine sediments from Novaya Zemlya. Sci Tot Env. 262:91-102. Carroll JL, Boisson F, Fowler SW, Teyssie JL. (1997) Radionuclide adsorption to sediments from nuclear waste dumping sites in the Kara Sea. Mar. Pollut. Bull. 1997; 35: 296-304. Carroll JL, Boisson F, Teyssie J-L, King SE, Krosshavn M, Carroll ML, Fowler SW, Povinec PP, Baxter MS. (1999) Distribution coefficients (Kds) for use in risk assessment models of the Kara Sea. Applied Radiation and Isotopes. 51:121-129. Dahlgaard H (1981) Bioindicators for monitoring radioactive pollution of the marine environment experiments on the feasibility of Mytilus as a bioindicator in estuarine environments with some comparisons to Fucus. Ris reports No. 15, Ris, Roskilde, Denmark 123 pp. Davis JA, Kent DB. (1990) Surface complexation modeling in aqueous geochemistry in Mineral-Water Interface Geochemistry: Reviews in mineralogy. Miner. Soc. Am. Washington, DC. 23: 177-260. Decho AW, Luoma SN. (1991) Time-courses in the retention of food material in the bivalves Potamocorbula amurensis and Macoma balthica: significance to the absorption of carbon and chromium. Marine Ecology Progress Series. 78:303-314.

Fisher NS, Fowler SW, Boisson F, Carroll J, Rissanen K, Salbu B, Sazykina TG, Sjoeblom KL. (1999) Radionuclide bioconcentration factors and sediment partition coefficients in Arctic Seas subject to contamination from dumped nuclear wastes. Environmental Science and Technology. 33:1979-1982. Gagnon C, Fisher NS (1997) The bioavailability of sediment-bound Cd, Co and Ag to the mussel Mytilus edulis. Can J Fish Aquat Sci 54:147-156. Hawkins AJS, Bayne BL, Bougrier S, Hral M, Iglesias JIP, Navarro E, Smith RFM, Urrutia MB. (1998) Some general relationships in comparing the feeding physiology of suspension-feeding bivalve molluscs. Journal of Experimental Marine Biology and Ecology 219:87-103. IAEA - International Atomic Energy Agency. (1985) Sediment Kds and concentration Factors for Radionuclides in the Marine Environment. Technical Reports Series No. 247, International Atomic Energy Agency, Wienna. 73 p. JRNC - Joint Russian-Norwegian Expert Group. (1997) Dumping of radioactive waste and investigation of radioactive contamination in the Kara Sea, 2nd edition, Report ISBN 82-993079-5-3. 55 pp. Landrum PF, Lee II H, Lydy MJ. (1992) Toxicokinetics in aquatic systems: Model comparisons and use in hazard assessment. Environmental Toxicology and Chemistry. 11:1709-1725. Luoma SN. (1983) Bioavailability of trace metals to aquatic organisms - a review. The Science of the Total Environment. 28:1-22. Oughton, D. H., B. Salbu, G. Riise, H. Lien, G. stby, A. Nren.Analyst, Vol. 117, March 1992, 481-486. Oughton, D.H., Brretzen, P., Salbu, B., Tronstad, E. (1997). Mobilisation of 137Cs and 90Sr from sediments: potential sources to arctic waters. The Science of the Total Environment. 202, 155-165. Salbu B (1985) Preconcentration and fractionation techniques in the determination of trace elements in natural waters their concentrations and physico-chemical forms. University of Oslo, Norway. Salbu, B., Nikitin, A.I., Strand, P., Christensen, G.C., Chumichev, V.B., Lind, B., Fjelldal, H., Bergan, T.D.S., Rudjord, A.L., Sickel, M., Valetova, N.K., Fyn, L. (1997). Radioactive contamination from dumped nuclear waste in the Kara Sea results from the joint Russian-Norwegian expeditions in the Kara Sea. The Science of the Total Environment. 202, 185-198. Skipperud L, Oughton DH, Salbu B (2000) The impact of plutonium speciation of the distribution coefficients in a sediment-seawater system, and radiological assessment of doses to humans. Health physics. 79:147-153. Spacie A, Hamelink JL (1982) Alternative models for describing the bioconcentration of organics in fish. Environ Toxicol Chem 1: 309-320. Tessier A, Campbell PGC, Bisson M. (1979) Sequential extraction procedure for the speciation of particulate trace metals. Analytical Chemistry. 51:844-851. Wang WX, Fisher NS, Luoma SN (1996) Kinetic determinations of trace element bioaccumulation in the mussel Mytilus edulis. Mar Ecol Prog Ser 140:91-113. Widdows J, Hawkins AJS (1989) Partitioning of rate of heat dissipation by Mytilus edulis into maintenance, feeding, and growth components. Physiol Zool 62:764-784. Yu-fu, Yu, B. Salbu, H. Bjrnstad, and H.N. Lien. Improvement of -energy resolution in determination of lowlevel Plutonium by liquid scintillation counting. J. Radioanal. Nucl. Chem. 145, 5, 345-353, 1990.

5. Radionuclide uptake and transfer in pelagic food chains of the Barents Sea.
Authors : Lars Fyn1, Hilde Elise Heldal1 and Per Varskog2
1 2

Institute of Marine Research, Bergen Institute for Energy Technology, Kjeller

5.1 Introduction
Impact assessments of contaminants in the marine environment have to be based both on their distributions and concentrations and knowledge of their behaviour in the marine environment. Contaminants may be partly dissolved, completely dissolved as ions, dispersed, bound to particles or bound in colloids. Some contaminants, in particular some organic persistent pollutants, have high lipid solubility and may therefore be stored in fat tissues of organisms at any trophic level. When stored in fat tissues, they are not easily available for metabolism, and transport from one trophic level to another may take place. Understanding various mechanisms for uptake and transport of contaminants through marine food webs or into marine organisms is complex and must be based on thorough knowledge of the main factors governing the presence of the actual contaminant in the marine environment. In the context of marine environmental radioactivity, there is a considerable lack of data, in particular when it comes to considering impact on different trophic levels. This is mainly due to the analytical complexity and the fact that the concentrations of most radionuclides in the marine environment are at the detection limit levels. For caesium-137 (137Cs) there are data, however scarce, which allow for some assessments. This study focuses therefore mainly on uptake and transport of 137Cs. 137Cs is one of the main components of radioactive wastes discharged into coastal waters of northwest Europe. The two most important terms for uptake and transport of contaminants in marine food webs are bioaccumulation and biomagnification. Bioaccumulation of a contaminant is uptake of the contaminant into the organism from both seawater and from dietary sources. Biomagnification is bioaccumulation of a contaminant resulting in increasing tissue concentrations of the contaminant as it passes from one trophic level to another. Trophic levels in pelagic food chains are generally organised as follows: Phytoplankton (primary producers) Zooplankton (secondary producers, primary consumers) Plankton eating fish (secondary consumers) Carnivorous fish and marine mammals (tertiary consumers)

Figure 5.1 illustrate the Barents Sea food web and its complexity, although simple compared to food webs at lower latitudes. The right hand side of Figure 5.1 represents

Man Sea birds

Piscivores

Polar bear

Seals

Whales Cod

Planktivores

Polar cod

Capelin; Herring

Herbivores

Ice fauna Copepods; Krill; Amphipods

Zooplankton Copepods; Krill; Amphipods; Ptreopods

Phytoplankton Ice algae; Other algae Diatoms Flagellates

Nutrients
Figure 5.1. The Barents Sea food web (after Dalpadado, 2000).

open waters while the left hand side represents the environment near the ice and at the iceedge. This study focuses on food webs in open waters (pelagic food webs). Large marine biota samples are normally required for radionuclide analysis. Sampling of enough phytoplankton in the field was found to be almost impossible by normal operational methods at sea. Therefore, uptake experiments of 137Cs and 57Co in five marine phytoplankton species representative for the Barents Sea phytoplankton community were carried out in the laboratory. The species studied were three prymnesiophytes, the coccolithophorid Emiliania huxleyi and the non-calcareous species Isochrysis galbana and Phaeocystis globosa, and two diatoms Skeletonema costatum and Thalassiosira pseudonana (Heldal et al., In press). 57Co was used as an analogue to 60Co, another important component of radioactive wastes discharged into coastal waters of northwest Europe. Co (cobalt) is essential to algae, and should therefore be taken up from seawater (Fogg, 1975).

In this study, zooplankton, the secondary producers, or the primary consumers, are represented by the copepod Calanus finmarchicus. C. finmarchicus is the main primary consumer in the Atlantic water mass of the Barents Sea (Melle & Skjoldal, 1998). Four different types of samples represent the zooplankton consumers, or the secondary consumers: Adult capelin (Mallotus villosus), herring (Clupea harengus), herring larvae of about 3 cm length and fry of saith (Pollachius virens) of about 4 6 cm length. They represent different steps in the community of zooplankton consumers as their sizes determine the size of the prey they can consume. For example, herring larvae will feed mostly on the early copepodit stages while adult herring feeds on krill, adult copepods and fish larvae. Cod (Gadus morhua) and harbour porpoises (Phocoena phocoena) represent the tertiary consumers.

5.2 Materials and methods

All samples except phytoplankton and harbour porpoises were collected during cruises conducted by the Institute of Marine Research (IMR) in 1998, 1999 and 2000. The uptake of 137Cs and 57Co in Emiliania huxleyi, Isochrysis galbana, Phaeocystis globosa, Skeletonema costatum and Thalassiosira pseudonana was studied in both growing and nongrowing cells over a six-day- and ten-day period, respectively. The details of the experimental set-up are given in Heldal et al. (In press). Zooplankton (Calanus finmarchicus) was collected using vertical tows at selected depth intervals by means of a WP-2 plankton net (56 cm opening, 180 m mesh size). The secondary consumers (adult capelin (Mallotus villosus), herring (Clupea harengus), herring larvae of about 3 cm length and fry of saith (Pollachius virens) of about 4 6 cm length were collected by means of pelagic trawl both in the intermediate waters and in surface waters. Cod (Gadus morhua) was collected by means of demersal trawl. Harbour porpoises (Phocoena phocoena) were collected opportunistically by commercial bottom-set gillnet fisheries along the Finnmark coast in northern Norway between April and June 1999. Nineteen porpoises were collected from this area, 8 females and 11 males. The methodical details are given in Tolley & Heldal (In press). With the exception of phytoplankton, all samples were carried deep-frozen to a land-based laboratory where the samples were subsequently ground, freeze dried, homogenized and filled into polyethylene counting boxes of appropriate size prior to analysis. The gamma counting for 137Cs was performed on a Canberra HP-Ge-detector with 30 % efficiency, an electric cryostat cooling system, and a 10 cm lead shielding. Concentration factors (CFs) were calculated by dividing the concentration of 137Cs in each species (Bq kg-1 ww (wet weight)) by the 137Cs concentration in seawater (Bq L-1). The 137Cs seawater concentration used were the median value of those available in the literature, 0.004 Bq L-1 (Kershaw et al., 1997; Grttheim, 1998).

5.3 Results and discussion

The main contributors to the present 137Cs contamination in the Barents Sea are the nuclear reprocessing industry in Europe and Chernobyl fallout, which drains through the Baltic Sea. The transport of radionuclides from south to north takes place within the different water masses of the current systems of the North Atlantic. A general view of the main currents is presented in Figure 5.2.

Figure 5.2. Depths and surface currents in the North Atlantic (green arrows = coastal waters, red arrows = Atlantic waters and blue arrows = Arctic waters).

The Norwegian Coastal Current (NCC) is the main transporter of radioactive contaminants, as NCC transports water entering the North Sea northwards until it gradually mixes with Atlantic water. Fyn & Svren (1997) found elevated levels of 137Cs in sediments close to Spitsbergen, an area with a more or less permanent Polarfront and a high primary production. The elevated levels of 137Cs was also found in relatively coarse sediments with a higher percentage of particles > 63 m. This is contrary to the common picture where radiocesium is bound to finer

(< 63 m) particles. Fyn & Svren (1997) suggested that phytoplankton in the water column in this area might act as scavenging elements and cause the elevated levels of 137Cs in sediments in the area. According to Heldal et al. (In press), the uptake of 137Cs in phytoplankton is low or even negligible. Their results indicate that phytoplankton are unlikely to influence the Cs build-up in marine food chains and Cs flux to deep waters. Figure 5.3 presents some of their results.
Em iliania huxleyi Isochrysis galbana Phaeo cystis globosa Skeletonema costatum Thalassio sira pseudonana a Bq Co-57/non-growing cell 1.2 10
-3

Bq C o-57/growing cell

1.2 10

-3

8.0 10

-4

8.0 10

-4

Bq Co-57/growing cece ll Bq Co-57/grow ing ll

4.0 10

-4

4.0 10

-4

0 0 0.0 10 0 50 10 0 hours 150 200 25 0 c

-4

0 0 0.0 10

-3 -3 E1000-40 a200 Emili a m 1.2 0rs0tonemaglobosa Th 0 -4 Ske leocy P150hrysis huxle atu Isoc 10ania a cpseudonana 1.2 Thalassiosira ost Ske P0 Isoc hae ostatum 8.0 alassi emra xle yia m 8.0 4.0haeton osihu cpseu donan a 4.0 5000le ocy astisglobosa 00.0i10anist isgalbana 0.0 1lihrysisgalbanyi hou 1550 2hours 250 0

50

hours

100

150 d

Bq Cs-137/non-growing cells

Bq C s-1 37/gro wing cells

3.0 10

3.0 10

-4

2.0 10

-4

2.0 10

-4

1.0 10

-4

1.0 10

-4

0 0 0.0 10

0 0 0.0 10

50

10 0

hours

150

200

250

50

hours

100

15 0

Figure 5.3. Uptake of 57Co and 137Cs in five phytoplankton species. a. Bq 57Co/cell, growing cells, b. Bq 57Co/cell, non-growing cells, c. Bq 137Cs/cell, growing cells, d. Bq 137Cs/cell, non-growing cells. (Heldal et al., In press)

As can be seen, there was no uptake of 137Cs in growing cells of any of the phytoplankton species (Fig. 5.3 c). For 57Co, there was a significant uptake in particular by Emiliana huxleyi (Fig. 5.3 a). Uptake of 57Co was expected; according to Fogg (1975) most algae need cobalt for their growth. Figure 5.3 b and d shows the uptake in non-growing cells for 57Co and 137Cs, respectively. There was a small accumulation of 57Co in all five species, and saturation was reached after approximately 100 hours. For 137Cs there was a pronounced variation for in particular Phaeocystis globosa, but the uptake was much lower than for 57Co, and no significant accumulation trend was observed. The accumulation and the variation in accumulation of 137Cs in non-growing cells may be explained by a variation in the state of the cells. Some may have been more degraded or gelated allowing for greater sorption, this process will also vary between species and even within the same species depending on the stage of development of the individual cells. Contrary to what was found for uptake in phytoplankton, 137Cs is bioaccumulated to a certain degree higher up in the food web. Table 5.1 shows concentrations of 137Cs and concentration factors (CFs) in different levels of the food chain. The zooplankton consumers herring, capelin, herring larvae and saith fry feed as mentioned on different components in the pelagic food webs, and all of them seem to bioaccumulate 137Cs. The calculated average CFs are 25 for these four planktivores (Table 5.1 (Heldal, unpublished data)). Since the same CF was

found for all zooplankton consumers, there are reasons to assume that there is an uptake of 137 Cs directly from seawater and not via the food web.
Table 5.1 : Concentration of 137Cs in different levels of the Barents Sea food web (Heldal, unpublished data). Bd = below detection limit, Concentration factor = (Bq kg-1 / Bq L-1); Estimated 137Cs concentration in seawater 0,004 Bq L-1

Specie
Calanus sp. Saith fry Herring larvae Capelin Herring

Bq kg-1 (wet weight) Bd 0,2 Bd 0,1 Bd 0,1 0,1 Bd 0,1

Concentration factor (CF) 50 25 25 25 25 125 73 - 148

Cod 0,5 Harbour porpoises 0,3 0,7

In this work, the secondary consumers, zooplankton, are represented by the copepod Calanus finmarchicus. Heldal (unpublished data) found a CF of 50 for C. finmarchicus (Table 5.1). This CF is twice the CF for the four representatives of the tertiary consumers. If biomagnification was taking place we should expect higher concentrations of 137Cs at least in adult herring and capelin due to the higher concentration of 137Cs in C. finmarchicus. However, due to small sample sizes and large uncertainties in the 137Cs measurements in C. finmarchicus, these results should be interpreted with some caution. Cod and harbour porpoises represent the next levels in the food web. The harbour porpoises analysed in the present study are part of a larger data set consisting of harbour porpoises sampled along the Norwegian coast from southern Norway (North Sea) to northern Norway (Barents Sea). The average concentration of 137Cs in porpoises decrease from southern Norway (3.8 Bq kg-1 (wet weight) to the Barents Sea (0.3 Bq kg-1 (wet weight)) (Tolley & Heldal (In press); Heldal & Tolley, 2001). The concentrations of 137Cs in porpoises are consistent with those found in seawater and sediments: the highest concentrations are found closest to the main sources for radioactive contamination: the Baltic Sea and reprocessing plants in northwest Europe. The concentrations of 137Cs in harbour porpoises sampled in the Barents Sea are at the same level as the concentrations in cod (Table 5.1). This further demonstrates a bioaccumulation with a CF for cod and harbour porpoise of 125 and 73 148, respectively, but no biomagnification. The results indicate uptake of 137Cs from seawater and not from dietary sources. Nevertheless, if uptake from dietary sources exists, there is also established an equilibrium between the organism and seawater, reflecting the concentration of 137Cs in seawater. Cesium is chemically equivalent to sodium (Na) and potassium (K) and both Na and K are totally dissolved in seawater as salt ions. Na and K are also essential for the ion-balance of the cells of organisms. If cesium is totally dissolved in seawater as a salt ion it is likely that

cesium ions will be part of the salt balance of the cells. In normal seawater with a salinity ~ 35, the non-radioactive isotope of cesium is present in a concentration of about 0,5 g L-1 and the amount of 137Cs in weight per volume is insignificant, i.e. the measured 137Cs concentration of 0,004 Bq L-1 represents about 1,2 x 10-10 g L-1. The salt ions of the radioactive and non-radioactive isotopes of cesium behave equally. Thus, uptake in an organism of non-radioactive and radioactive cesium is likely to take place in the same proportions on a weight basis as they are found in seawater.

5.4 Conclusion
Bioaccumulation of 137Cs is not observed in growing cells of five phytoplankton species representing the Barents Sea phytoplankton community. Bioaccumulation is, however, observed in organisms representing higher levels in the Barents Sea food webs. Our results indicate a direct uptake of 137Cs from seawater. A transport of 137Cs upward through the Barents Sea food web (biomagnification) does not seem to take place.

References
Dalpadado, P. (2000). The Barents Sea food web. In Fyn, L. (ed). Environmental Impact and Fisheries. TemaNord 2000:583. Nordic Council of Ministers, Copenhagen 2000. ISBN 92-893-0519-3. ISSN 0908-6692, pp 17-29. Fogg, G. E. (1975). Primary productivity. In Riley, J. P. and Skirrow, G. (eds). Chemical Oceanography. Volume 2, 2nd edition. Academic Press 1975, pp 385-453. Fyn, L. & Svren, I. (1997). Distribution and sedimentation of radionuclides in the Barents Sea. ICES Journal of Marine Sciences; 54: 333-340. Grttheim, S. (1998). A preliminary report on radioactive contamination in the northern marine environment. Studies on distribution of radiocaesium, plutonium and americium in seawater and sediments (M.Sc. Thesis). Norwegian Radiation Protection Authority and Biological Institute, University of Oslo, Norway Heldal, H. E. & Tolley, K. A. (2001). Regional differences in radioactive caesium in harbour porpoises (Phocoena phocoena), Poster, Miljkjemisk Vintermte, Hafjell, 31. Jan-03. Feb., 2001. Heldal, H. E., Stupakoff, I. and Fisher, N. S. (In press). Bioaccumulation of phytplankton species. Journal of Environmental Radioactivity.
137

Cs and

57

Co by five marine

Kershaw PJ, Gurbutt P, Woodhead D, Leonard K, Rees J (1997). Estimates of fluxes of 137Cs in northern waters from recent measurements. The Science of the Total Environment; 202:211-223. Melle W. & Skjoldal H.R. (1998). Reproduction and development of Calanus finmarchicus, C. glacialis and C. hyperboreus in the Barents Sea. Marine Ecology Progress Series; 169: 211-228. Tolley, K. A. & Heldal, H. E. (In press). Inferring ecological separation from regional differences in radioactive caesium in harbour porpoises (Phocoena phocoena). Marine Ecology Progress Series.

6. Ecological dosimetry models

Authors : Ivan Kryshev1, Tatiana Sazykina1, A. Kryshev1, Justin Brown2
1 2

SPA TYPHOON Norwegian Radiation Protection Authority

6.1 TYPHOON methodology

Under natural conditions, organisms are exposed to various sources of ionizing radiation. Absorbed dose to hydrobionts depends on a number of factors. Among them are type and energy of emitters (photons, beta particles, alpha particles, protons, neutrons, etc.), radiation source geometry (point or extended), space distribution and time evolution of radionuclide concentrations in components of aquatic ecosystems, ecologicalphysiological parameters and stage of ontogenesis of the organism (IAEA, 1976, 1979; Kryshev & Sazykina, 1986, 1990, 1995; Amiro, 1997; Sazykina et al., 1998). In the general case, the assessment of doses to organisms is an intricate problem. For the sake of simplicity, the dose rate assessments, as a rule, will be presented below for uniform distribution of radionuclides throughout the volume of organisms (for incorporated emitters) or environment (in calculations of external exposure).

6.1.1 Radiation dose from incorporated radionuclides

An important characteristic in calculations of internal dose is the relation between linear dimensions of the organisms and the maximum path lengths of ionizing particles in tissues (IAEA, 1976; Kryshev & Sazykina, 1986, 1990). This characteristic enables one to estimate the contribution of alpha, beta and gamma radiation sources. For phytoplankton with cell dimensions of no more than several hundreds of micrometers, a major contribution to internal dose can be due to alpha particles with a maximum path length of the order of several tens of micrometers. The energy of beta particles with a path length of several millimeters in a medium of unit density dissipates mostly outside of the organism. In calculations of internal exposure of microalgae, the contribution of gamma emitters can be neglected. In spite of the fact that the cells of phytoplankton take a great variety of shapes, they can be approximated to spheres in dose assessments owing to their small dimensions. For the organisms of zooplankton with average dimensions ranging from 0.1 cm to 1.0 cm, the dose rate from alpha emitters is equal to P , i.e. to the dose rate in an infinite volume uniformly filled with a radionuclide with a specific concentration identical to that in the hydrobiont. In calculations of exposure from incorporated beta sources and gamma emitters, it is necessary to take into account geometric parameters. For large organisms such as mollusks, crustaceans, fish and macroalgae, the contributions to the dose rate due to alpha and beta emitters is taken to be equal to P and P . Consequently, the effects associated with finite dimensions of large hydrobionts become negligible for these

emitters but remain important for absorption of gamma radiation. In some cases, there is a need to calculate dose loads on individual organs or tissues of large hydrobionts. 6.1.1.1 Assessment of dose from incorporated alpha emitters If the dimensions of a hydrobiont are large compared to the path length of alpha particles, the dose rate to the hydrobiont is approximately equal to the specific dose rate created in the infinite volume of an absorbing material, within which the radionuclide is uniformly distributed. The radionuclide concentration y (Bq/g of the absorber mass) corresponds to the emitter content in the hydrobiont tissues. The values of P (nGy/s) can be found using the following formula: P = 0.16 E y
where : E is the average energy of alpha particle per decay (Mev).

6.1

For small spherical volumes the dose rate can be calculated with the formula P =
r

l r

P = 0.75

r r

6.2

where : l = 0.75 r is the mean path length of alpha particles emitted inside a sphere of radius r within this sphere; r is the mean path length of alpha particle of the given energy E in a biological tissue (Table 6.1). Table 6.1. The path lengths of alpha particles in the air and biological tissue in relation to the energy of particles
Energy of alpha particles (Mev) 4.0 4.5 5.0 5.5 6.0 6.5 7.0 7.5 8.0 9.0 10.0 Air (cm) 2.37 2.82 3.29 3.82 4.60 4.96 5.58 6.23 7.19 8.56 10.20 Biological tissue (m) 26.2 31.2 36.7 42.6 48.8 55.5 62.4 69.9 78.0 94.4 112.0

6.1.1.2 Assessment of dose from incorporated beta emitters The distribution of dose within small-sized organisms can be obtained by appropriate integration of the dose function of a point source. Providing that the radioactive material is uniformly distributed throughout a sphere, and this sphere is surrounded by an absorber of the same composition and density, the dose rate at the center of a spherical source of beta particles is given by the following expression (Equation 6.3): Psph (0, r ) = P {c 2 [r / c + (1 + r / c) exp(1 r / c) 3] + 1 (1 + r ) exp(1 r )} 6.3

where : r is the radius of the sphere (cm); and c are parameters presented in Table 6.2 for selected radionuclides; P is the dose within a large source of beta particles with the radionuclide concentration identical to that in the sphere (Equation 6.4).

P = 0.16 E y
where : E is the average energy; y is the concentration of beta emitter, Bq/g.

6.4

For small sphere radii (r << 1), Equation 6.3 may be simplified substantially to take the form (Equation 6.5) :

Psph (0, r ) P cr

6.5

where : ,c and are shown in Table 6.2 for selected radionuclides; r is the radius of the sphere (cm).

The -radiation dose rate distribution in hydrobionts of arbitrary shape is rather difficult to determine by direct integration of the dose function. Consequently, in TYPHOON calculations, organisms are approximated by spheres and fragments of spherical layers, as well as by plane blocks of finite thickness and other elementary spherical figures. Some parameters of beta-emitting radionuclides, which are required for assessments of doses to the organisms, are given in Table 6.2.
Table 6.2. Characteristics of beta-emitting radionuclides
Radionuclide 3 H 14 C 32 P 40 K 60 Co 90 Sr 90 Y 99 Tc 134 Cs T1/2 12.34 year 5730 years 14.3 days 1.28 109 years 5.25 years 28.6 years 2.68 days 2.13 105 years 2.07 years E0, Mev 0.0186 0.155 1.71 1.314 0.318 0.546 2.274 0.292 0.089 0.415 0.658 0.512 1.173

137

Cs

30.17 years

E , Mev/decay 0.00571 0.0493 0.694 0.445 0.0963 0.196 0.928 0.101 0.006 0.003 0.147 0.157 0.165 0.015 0.180

, cm2/g 13100 357 9.20 9.42 105 38.8 6.20 122 900 66.7 30.5
46.6 11.4

c 3.11 2.65 1.11 1.22 2.05 1.70 1.00 2.11 3.11 1.86 1.57 1.72 1.27

0.184 0.213 0.326 0.319 0.257 0.285 0.333 0.252 0.184 0.271 0.292
0.281 0.315

6.1.1.3. Gamma radiation doses from incorporated radionuclides In practice, the average dose rate from incorporated gamma emitters is calculated using the following relationship (Equation 6.6) :

P = 1.1454 y g 10 5
6.6 where : is the -radiation constant of the raidonuclide in aGy m2/ (s Bq) (Table 6.5); g is the average geometric factor which is determined as follows (Equation 6.7):

g=

1 V

dV

6.7

The geometric factors at the center of spheres of varying dimensions are presented in Table 6.3. These data can be used to calculate g using Equation 6.8.
Table 6.3. The values of the geometric factor at the centers of the sphere for assessments of the doserate from gamma radiation
Radius of the sphere, r, cm 1 2 3 4 6 8 10 g0, cm 12.6 25.2 37.8 50.4 75.6 101 126

For the sphere, the average dose rate throughout the spherical volume accounts for 0.75 of the dose rate at the center of the sphere, i.e. 3 g sph = g 0 6.8 4 To a good approximation, at r < 10 cm g sph = 3r The average geometric factor for cylinders of different size is given in Table 6.4.
Table 6.4. The average geometric factor for cylinders with a uniformly distributed gamma-active nuclide

6.9

Height of the
cylinder, cm 2 5 10 20 30 40 60 80 100

Radius of the cylinder, cm

3 17.5 22.3 25.1 25.7 25.9 25.9 26.0 26.0 26.0 5 22.1 31.8 38.1 40.5 41.0 41.3 41.6 41.6 41.6 10 30.3 47.7 61.3 68.9 71.3 72.4 73.0 73.8 73.8 15 34.0 56.4 76.1 89.8 94.6 96.5 97.8 98.4 98.5 20 36.2 61.6 86.5 105 112 116 118 119 119 25 37.5 65.2 93.4 117 126 131 134 135 136 30 38.6 67.9 98.4 126 137 143 148 150 150 35 39.3 70.5 103 133 146 153 159 161 162

In some cases, particularly for aquatic organisms relatively large in size (with linear dimensions of the order of tens of centimeters and over), the scattered radiation of gamma quanta must be taken into account. Neglecting the effect of scattering may lead to underestimation of doses from gamma emitters by a factor of 3-5. To take into account the accumulation factor of scattered radiation, the following Equations (6.10-6.12) can be applied. 4 1.11 y A1 1 A1 P = ( + ) S 1 1 1 + 2 6.10

where : P is the dose-rate in an infinite source with a uniformly distributed -emitter; is the
radiation constant of the radionuclide in aGy m2/ (s Bq) A1, 1 and 2 coefficients in the Taylor representation of the accumulation factor of scattered radiation in water, s is the linear coefficient of gamma quanta attenuation in the solid which can be approximated as that for water in the case of biota. All terms are presented in Table 6.5.

P ( z ) = P 0.5 P [ E2 ( s z ) + E2 ( S (h z ))]
where :

6.11

P ( z ) is the dose rate at distance z (cm) from the surface; h is the thickness of the layer (cm) and E is defined in Equation 6.12 below :
2

E 2 ( S z) =

A1 1 A1 E 2 ( S (1 1 ) z ) + E 2 ( S (1 + 2 ) z ) 11 1+ 2

6.12

There are other ways of taking into account the effects of gamma quantum scattering as well. The factors of scattering for radiation sources of different geometry are given in (Mashkovich, 1982; Foderato & Hall, 1981; Kryshev & Sazykina, 1990).
Table 6.5. Characteristics of gamma-emitting nuclides
Radionuclide 40 K 60 Co
65

T1/2 1.28 109 years 5.25 years 245 days 2.07 years

Zn Cs

134

137

Cs

30.17 years

, aGy m2/(s Bq) 5.10 44.42 40.21 84.63 19.57 0.55 20.12 27.38 22.17 5.00 57.44 21.00 0.33 21.33

, 1/cm 0.0585 0.064 0.066

0.0680 0.0976 0.0796 0.0904 0.0900 0.0867 0.3210

A1 856.6 768.3 685.3 648.9 2637 2775 3271 3271 3122 8.5

1 0.0216 0.0235 0.0311

0.0331 0.0665 0.0435 0.0570 0.0570 0.0530 0.0374

2 -0.0203 -0.0248 -0.0290

-0.0309 -0.0657 -0.0433 -0.0564 -0.0564 -0.0525 0.1157

* Note. The following symbols are used in the table: T1/2 - half-life; - gamma radiation constant; linear coefficient of gamma quanta attenuation in water; A 1, 1, 2 - coefficients in the Taylor representation of the accumulation factor of scattered radiation in water.

6.1.2 Radiation doses from external sources

6.1.2.1 Exposure from water The dose rates to aquatic organisms from alpha and beta emitters scattered in the water depth are calculated with the following formulas: P ,W = P P ( F ) V P ,W = P P ( F ) V

6.13

where P and P are calculated with the Equations 6.1 and 6.4, whereas P(F)v and P(F)v characterize the dose rates in the area occupied by the organism. All these quantities are determined from the radionuclide concentration in water. Considering the water depth as the infinite source with a uniformly distributed -emitter, we can write for the external gamma-radiation dose rate to hydrobionts (Equation 6.14) PW = P 6.14
where :

10 5 P = 4 1.11 y 6.15 s where is the gamma radiation constant of a radionuclide, aGy m2 / (s Bq); y is the concentration of the radionuclide, Bq/dm3; s is the gamma radiation attenuation factor, 1/cm.

P is calculated with the formula (6.15) from the radionuclide concentration in water. At small depths of a water body the external gamma-radiation dose rate can be calculated using a well-known relationship for the determination of the gamma radiation field from a source in the form of a shielded sheet (6.16) : PW = 0.5P [ E 2 ( S z ) E 2 ( S ( z + h))] 6.16

where h is the water layer depth, cm; z is the shielding layer depth determined by the dimensions of organisms, cm; P is calculated with Equation 6.15 from the radionuclide concentration in water; E2(s z) is calculated using Equation 6.12. 6.1.2.2 Exposure from bottom sediments In many cases, when exposure to aquatic organisms nearby the surface of bottom sediments is considered, the sediments can be represented as an infinitely thick source with a uniformly distributed activity. In these cases, the beta- and gamma-radiation dose rates nearby the surface of bottom sediments are equal to 0.5 P and 0.5 P, respectively. In the general case, as radionuclides are non-uniformly distributed in bottom sediments, the external gamma-radiation dose rate from the sediments to the organisms can be calculated with the formulas similar to Equation 6.16.

6.1.2.3 Exposure from other organisms External exposure to gamma radiation from clusters of macroalgae can be calculated using Equation 6.16. In this case, h is the alga layer thickness; z is the thickness of a water layer separating the exposed organism from the surface of algae. The value of P is calculated from the radionuclide content in algae. The exposure from aquatic plants may be a significant radioecological factor for phytophilous species of fish spawning in the overgrowing aquatic vegetation. Fish embryos may be exposed to additional external irradiation when fish eggs form clusters. In practice, dosimetric calculations require information on the mutual arrangement of fish eggs in clusters (hexagonal close packing, aggregation in clots, etc.). Account must be taken of the shielding against exposure from water provided by fish eggs.

6.1.3 Formalised algorithms

TYPHOON use the FORTRAN programme DOSBIO (doses to marine biota in the Arctic Seas) for systemization of the algorithms presented above.

6.2 NRPA methodology

It is convenient in absorbed dose calculations to use an equilibrium absorbed dose constant, which equates to the total energy emitted by individual components, i, of electromagnetic and/or particulate radiations after the decay of a specific radionuclide (Brownell et al., 1968). If it is assumed that a radionuclide is uniformly distributed throughout the body of an organism and that all the energy emitted by this radionuclide, during radioactive decay, is transferred to the organism, the absorbed dose rate to the biota can be defined by Equation 6.17. D = 5.04 10 6 A E i yi
i .

6.17

where :

A= Activity concentration (Bq kg-1 w.w.) Ei = Energy emitted by component i of (,, )radiation yi = fractional abundance or yield of radiation particles/photons of energy Ei 5.04 x 10-6 = Factor to account for conversions of MeV to Joules (1 MeV = 1.602 x 10-13 J) and seconds to years (1 year = 3.145 x 107 seconds),

D=

Dose rate (Gy a-1)

In a situation where the calculation of internal doses to biota arising from radionuclides (assumed to be uniformly distributed throughout the body), is required for radiations that have short ranges in environmental media, e.g. low energy - and -particles, then Equation 6.17 should provide a reasonable estimate of the absorbed dose rate. In situations where the absorption mean free path is high relative to the dimensions of the organism, or components of an organism, being considered, e.g. medium-high energy photons, then account should ideally be taken of the fact that only a fraction of the energy released, during each decay, is absorbed by the organism. For photons, the energy transferred to the target can be calculated, quite simply, by the application of an absorbed fraction, , defined as the fraction of the

emitted photon energy absorbed in the region of interest (Brownell et al., 1968). This term is expressed in Equation 6.18.

photon energy absorbed by target photon energy emitted by source

6.18

A modified version of Equation 6.17, which takes account of the fact that not all the emitted photon energy is absorbed by the organism can be written thus (Equation 6.19) : D = 5.04 10 6 A i E i yi
i .

6.19

where :

Dose rate (Gy a-1) A = Activity concentration (Bq kg-1 w.w.) Ei = Energy of component i of gamma spectrum yi = Fractional abundance or yield of radiation photons of energy Ei i = Absorbed fraction for energy Ei
D =

A computer model has been developed to calculate internal doses to biota arising from the anthropogenic radionuclides 137Cs, 90Sr, 99Tc, 238Pu, 239,240Pu, 241Am and the natural (and in some cases technologically-enhanced) radionuclides 40K and 210Po, using the algorithms outlined above. All radionuclide data have been derived from ICRP Publication 38 (ICRP, 1983). External doses are also calculated using the dose conversion factors tabulated by Amiro (1997). The models (written in Microsoft Visual Basic) runs in the Microsoft Excel environment. Examples of dialogue boxes are presented in Figure 6.1.

Figure 6.1 : Examples of dialogue boxes in the aquatic dosimetry model.

6.3 Biota doses derived from archived data

6.3.1 TYPHOON study
The estimated doses for the biota of the Barents and Kara Seas obtained on the basis of actual radiooactivity levels in components of the marine ecosystem are presented in Table 6.6 (Kryshev & Sazykina, 1995). The results are based on input data (activity concentrations in environmental media) from TYPHOON archives. It is seen from this table that for Arctic marine biota the additional doses from artificial radionuclides considerably lower than the natural background radiation.
Table 6.6. The estimated internal exposures for Arctic marine biota, 10-9 Gy/day (mGy/a)

Marine biota Crustaceans Mollusks Fish

Barents Sea 2 (7.3 x 10-4) 3 (1.1 x 10-3) 20 (7.3 x 10-3)

Kara Sea 3 (1.1 x 10-3) 5 (1.8 x 10-3) 30 (1.1 x 10-2)

Natural background 3500 (1.27) 2700 (0.98) 800 (0.3)

6.3.2 NRPA study

6.3.2.1 Data collation Data sets exist providing information on activity concentrations in environmental samples taken in the 1990s from Norwegian coastal waters (Brungot et al., 1997; Brungot et al., 1999), however knowledge gaps are evident. Owing to this lack of data in certain areas, information was derived from other studies (MAFF, 1994; MAFF, 1996) and, in some cases, the use of generic concentration factors (IAEA, 1985) where sea water concentrations only were known. These data are presented in Table 6.7.
Table 6.7 : Activity levels (Bq kg-1, w.w.) for biota, sea water (Bq m-3) and sediment (Bq kg-1 d.w.) in Norwegian coastal waters used for input into biota dose model.
137 90 99 238 239,240 210 40 Biota Cs a Sr c Tc a Pu a,d Pu a,d 241Am a,d Po e Ke -4 -4 -4 Lobster 0.9 0.75 38.5 5 x 10 7 x 10 5 x 10 17 70 Mussels 0.08 2.6 0.5 5 x 10-3 7 x 10-3 0.02 60 70 Seaweed 0.5 a,b 4.1 44.5 3 x 10-3 4.5 x 10-3 8 x 10-3 0.35 400 Sea water 11.4 3.5 f 5d 1.6 x 10-3 a 2.2 x 10-3 a 1 x 10-3 a 1 x 10-3 11x103 * d -3 a -3 a -3 a Sediment 1.9 3.5 0.5 0.27 x 10 2.8 x 10 0.8 x 10 20 * 500 * a data (1997) from Norwegian national surveillance report (Brungot et al., 1999); b dry weight measurement was 2.7 Bq kg-1, converted to wet weight by multiplying by 0.2 (IAEA, 1985); c data from MAFF (1996); d CFs/kds (IAEA, 1985) applied to sea water concentrations; e data from MAFF (1994); f 1993-1995 data - Brungot et al. (1997); * estimated - silty sediments.

The model allows for variations in geometry (applied to gamma emissions only) and in habitat (four categories : pelagic, demersal, benthic and sediment-dwelling). Lobsters were represented by a 1 kg sphere/thick ellipsoid living on the sea bed (benthic), mussels as a 10 g small ellipsoid (surrounded by scattering medium) living on the sea bed and seaweed as a benthic 1 kg sphere/thick ellipsoid.

6.3.2.2 Results Total doses (internal and external) were calculated from model runs and results are presented in Figures 6.2-6.4.
Dose = 1.35 mGy a-1
Tc-99 1.5 % Po-210 34%

Dose = 2.5 mGy a-1

Others <1% K-40 34% Po-210 66%

K-40 64%

Figure 6.2 : Total doses to lobster

Dose = 1.8 mGy a-1
Po-210 <0.5 %

Figure 6.3 : Total doses to mussels

Others <2 %

K-40 98%

Figure 6.4 : Total doses to seaweed

For the suite of radionuclides considered, total doses varied between 1.35 mGy a -1 and 2.5 mGy a-1. The doses were essentially attributable to the natural radionuclides 40K and 210Po. For mussels and seaweed, the internal component of the dose was predominant, forming 73 % and 62 % of the total dose respectively, whereas for lobster, the external component and internal component were of equal magnitude. In terms of the anthropogenic radionuclides, 99Tc was the most important dose-forming radionuclide for lobsters and seaweed. Doses arising from 99 Tc were calculated as 20 Gy a-1 for lobster and 23 Gy a-1 for seaweed almost entirely attributable to the internal component of dose. It is also worth commenting on the application of absorbed fractions to dose calculations. In an earlier study by the authors of this article (Brown et al., in press) internal doses were calculated using equilibrium absorbed dose constants where it is assumed that all energies emitted by the selected radionuclides are absorbed by the target (Equation 6.17). Using the modified equation (Equation 6.19) leads to a reduction in the calculated internal dose by up to 20 % dependent on the importance of gamma-emitting radionuclides in the dose formation. For example, the internal dose arising from the suite of radionuclides considered was calculated as 1.415 mGy a-1 for seaweed using the old method compared to an internal dose of 1.14 mGy a-1 using the new method.

6.3.3 Combined results

Although the dose rates derived from the TYPHOON and NRPA studies are (i) for different locations, i.e. Kara and Barents Sea in the case of the TYPHOON study, Norwegian coastal environments for the NRPA study, and (ii) for internal doses only in the case of the TYPHOON study and for internal + external doses in the case of the NRPA study, the total calculated doses are of a similar magnitude. In both studies, naturally-occurring radionuclides are shown to contribute very significantly to the dose-rate. An interesting point relates to the fact that the internal dose rate for biota arising from anthropogenic radionuclides in Norwegian coastal waters (in particular the south and west coasts) may be slightly higher than the corresponding dose rates observed in the Barents Sea mainly because of the higher levels of 99Tc observed in the biota tissue sampled in more southerly locations.

6.4 Biota doses derived from the Barents Sea expedition 1999 NRPA
6.4.1 Input data
The bottom water and surface (0-2 cm) sediment activity concentrations from Station 3 were used as input data for the external dose models. Internal dose calculations were conducted using the activity concentrations measured either in body tissue or the whole organism of shrimp (Pandalus borealis) from Trawl Station 44. These data are summarised in Table 6.8.
Table 6.8 : Activity concentrations from environmental samples taken during the Barents 1999 expedition and used for input to biota dosimetric models
Sample Activity concentrations 137 99 90 239,240 Cs Tc Sr Pu -3 -3 -3 a Water 3.41 Bq m 0.54 Bq m 1.65 Bq m 13.7 mBq m-3 Sediment 4.7 Bq kg-1 d.w. n.d. 0.61 Bq kg-1 d.w. 0.032 Bq kg-1 d.w. -1 -1 b Shrimp 0.08 Bq kg w.w. 0.075 Bq kg w.w. 0.018 n.d. a surface water activity; b converted to wet weight using an assumed dry weight/wet weight ratio of 1:4. Assumed that activity concentration was at the detection limit.

It should be noted that absorbed doses for the artificial radionuclides 137Cs, 90Sr, 99Tc and 239,240 Pu only have been calculated. In the case of 239,240Pu internal doses were not included and in the case of 99Tc external doses were not included for lack of analysis data. The shrimp was represented by a 1 g small ellipsoid (surrounded by scattering medium). The shrimp was assumed to inhabit the demersal zone where exposure from the water column dominated. The total external exposure is calculated by (arbitrarily) weighting the exposure from water by a factor of 0.75 and the exposure from sediment by 0.25 in attempt to account for exposure from combined sources.

Table 6.9. Results from dose rate calculations for shrimp in the Barents Sea. Radionculide
Internal dose rate (Gy/y)
137 90 99

External dose rate (Gy/y) 4,73 x 10-6 7,07 x 10-8 3,49 x 10-11 a 5,30 x 10-11 4,80 x 10-6

Int + ext dose rate (Gy/y) 4,81 x 10-6 8,84 x 10-8 3,83 x 10-8 5,30 x 10-11 4,94 x 10-6

Cs

8,19 x 10-8 1,77 x 10-8 3,83 x 10-8

Sr Tc Pu

239,240

n.d 1,38 x 10-7

Total
a

external dose from water only; n.d. not determined

The total dose rate is extremely low amounting to approximately 5 Gy/year (Table 6.9). A large proportion of the dose rate is derived from the external irradiation of the shrimp from 137 Cs (note the component is effectively from daughter radionuclide 137mBa) in bottom water and sediments.

6.5 Biota doses derived from release scenarios TYPHOON

Doses to marine organisms inhabiting the RW dumping sites in the bays of Novaya Zemlya were calculated using predicted levels of future environmental contamination, associated with potential radionuclide releases from the containers with radioactive materials (Sazykina et al., 1998).

6.5.1 Release scenario

Model scenarios for the potential radionuclide releases patterns from the dumped containers with radioactive materials were developed within the framework of the International Arctic Seas Assessment Project (IASAP in the period 1993-1996) under the auspices of the International Atomic Energy Agency (Sjoblom & Linsley, 1995; Lynn et al., 1995). These IASAP source term scenarios provided predictions of annual release rates for a wide set of radionuclides from each site of RW dumpings over the period of 1000 years in the future. To evaluate the highest potential doses to marine biota, the release rates predicted for the socalled plausible worst case scenario were used, based on the assumption of an accidental disruption in 2050 AD of dumped fuel containers in the Tsivolki Fjord, with a release spike of 110,000 GBq followed by much smaller releases in the subsequent years.

6.5.2 Results : Potential doses to marine biota in the Tsivolki Fjord (Realisation of the IASAP Scenario)
The highest levels of radioactive contamination of the fjord are expected in the case of realization of the so-called plausible worst case scenario developed by the IASAP experts. The calculated concentrations of the most important radionuclides in water and bottom sediments of the Tsivolki Fjord during the period of highest releases (2050-2055 AD) are given in Table 6.10 (Sazykina et al., 1998).

Table 6.10. Predicted levels of radionuclide concentrations in the Tsivolki Fjord in the case of realization of the IASAP plausible worst case scenario (Sazykina et al., 1998)

Radionuclide Year 137 Cs 90 Sr 63 Ni 239 Pu 240 Pu 241 Am

Water, Bq/m3 2050 AD 0.42E+05 0.37E+05 0.11E+05 0.14E+04 0.62E+03 0.28E+03

2055 AD 0.32E+04 0.28E+04 0.15E+05 0.37E+02 0.16E+02 0.26E+01

Sediments (0-5 cm), Bq/kg dw 2050 AD 2055 AD 0.17E+03 0.64E+03 0.49E+02 0.19E+03 0.12E+05 0.21E+05 0.11E+03 0.36E+03 0.49E+02 0.16E+03 0.49E+02 0.12E+03

The calculated dose rates to different types of marine biota are presented in Table 6.11. Because of the presence of great amounts of actinides in the releases, their contribution to potential dose rates predominates (Table 6.12). The contribution of internal exposure to the total dose rate for all types of organisms is greater than 90 %.
Table 6.11. Predicted dose rates to marine biota in the Tsivolki Fjord in the case of realization of the IASAP plausible worst case scenario

Organism/year Mollusk Small fish Big fish Sea mammal

Total dose rate, mSv h-1 2050 AD 0.4 0.0065 0.0067 0.0068

2055 AD 0.01 0.0004 0.0004 0.0004

Table 6.12. The percentage contribution of different radionuclides to the expected doses to the local marine biota during the year of highest releases (2050 AD, Tsivolki Fjord)

Organism Mollusk Small fish Big fish Sea mammal

Actinides 99.88 87.7 86 83.6

Fission products 0.07 10.8 12.6 15

Activation products 0.05 1.5 1.4 1.4

6.6 Interpretation of results in terms of dose-effects relationships.

The question of what constitutes damage to the environment is not a simple matter. Traditionally, protection criteria have been based on protection of populations of wild plants and animals (IAEA, 1992; UNSCEAR, 1996) but the fact that the law in some countries

protects individuals of certain species, e.g. endangered species, renders the topic of protection of individual versus population open for debate (IAEA, 2000). In relation to effects on populations, a general conclusion of IAEA Technical Report 332 (IAEA, 1992) was that in aquatic environments, limiting chronic dose-rates to 10 mGy/day or less to the maximally exposed individuals in the population would provide adequate protection for the population. With respect to effects of radiation at the individual level, numerous possible end-points exist including death, fertility, fecundity and scorable cytogenetic damage. Effects on reproduction may be an end point of interest owing to the repercussions that any damage to reproductive capability may have on the long-term viability of biota populations. In other words, this end point will provide information both on the well being of an individual and the health of a population as a whole. In relation to specific reproduction damage in individuals, a relevant conclusion from UNSCEAR (1996) was that a dose rate of less than 1 mGy per hour is unlikely to produce significant effects in the gonads of fish. In all situations, ranging from calculations based on monitoring data through to calculations based on release scenarios, dose-rates derived from artificial radionuclides are below the levels where effects from ionising radiation would be observable upon the reproductive capability of individuals (specifically fish in this case) or populations of aquatic species. Having said this, large knowledge gaps do exist in relation to dose-effect relationships for numerous marine species which restricts the conclusions made at the present time to generalisations and extrapolations based on the dose-response data we do have.

References

Amiro, B.D. (1997). Radiological dose conversion factors for generic non-human biota used for screening potential ecological impacts. J.of Environmental Radioactivity, 35, 37-51. Brown, J.E., Strand, P. & Bergan, T.D.S. (in press). Doses to biota arising from the increased levels of 99Tc in Norwegian coastal waters. Second International Symposium on Ionising radiation. Ottawa, 10-14th May, 1999. Brownell, G.L., Ellet, W.H. & Reddy, A.R. (1968). Absorbed fractions for photon dosimetry Journal of Nuclear Medicine, 9, pp27-39. Brungot, A.L., Sickel, M.A., Bergan, T.D., Be B., Hellstrm, T. & Strand, P. (1997). Radioactivity in the marine environment. Report no 2 from the national surveillance Programme.StrlevernRapport 1997:3. Norwegian Radiation Protection Authority, sters, Norway. Brungot, A.L., Fyn L., Caroll, J., A-K. Kolstad, Brown, J.E., Rudjord, A-L., Be, B. & Hellstrm, T. (1999). Radioactivity in the marine environment. Report no 3 from the national surveillance Programme.StrlevernRapport 1999:6. Norwegian Radiation Protection Authority, sters, Norway. Foderato, A. And Hall, R.J. (1981). Application of three-exponential representation of photon buildup factors to water. Nucl. Sci. Eng. Vol.78 (1), 74-78. IAEA - International Atomic Energy Agency (1976). Woodhead, D.S. Concentrations of Radionuclides In Aquatic Environments and the Resultant Radiation Dose Rates Received by Aquatic Organisms. In: Effects of Ionizing Radiation Dose Rates Received by Aquatic Organisms and Ecosystems. Vienna: IAEA, tech.rep.ser. No.172, 5-54. IAEA - International Atomic Energy Agency (1979). Woodhead D.S. Methods of dosimetry for aquatic organisms. In: Methodology for assessing impacts of radioactivity on aquatic organisms. Vienna, Tech. rep. ser. N 190, 43-96.

IAEA. (1985).Sediment kds and concentration factors for radionuclides in the marine environment. International Atomic Energy Agency, IAEA Technical Report Series No. 247. International Atomic Energy Agency, (IAEA, Vienna). IAEA (1992). Effects of ionising radiation on plants and animals at levels implied by current radiation protection standards. IAEA Technical Report Series No. 332. International Atomic Energy Agency, (IAEA, Vienna). IAEA (2000). Protection of the environment form the effects of ionising radiation : A report for discussion. IAEA-TECDOC-1091. International Atomic Energy Agency, (IAEA, Vienna). ICRP. Radionuclide transformations. Energy and intensity of emissions. ICRP Publication 38. Annals of the ICRP, 11-13, Pergammon Press (Oxford) (1983). Kryshev, I.I. and Sazykina, T.G. (1986). Mathematical modelling of radionuclide migration in aquatic ecosystems. Moscow, Publ. House Energoatomizdat (in Russian). Kryshev I.I., Sazykina T.G. (1990). Simulation Models for the Dynamics of Ecosystems under Conditions of the Anthropogenic Impact of TPP and NPP. Moscow: Energoatomizdat (in Russian). Kryshev, I.I. and Sazykina, T.G. (1995). Radiological Consequences of Radioactive Contamination of the Kara and Barents Seas. J. of Environmental Radioactivity, Vol.29, N 3, p.213-223. Lynn, N., Timms, S., Warden, J. et al. (1995). Scenarios for Potential Radionuclide Release from Marine Reactors Dumped in the Kara Sea. In: Environmental Radioactivity in the Arctic. Eds.:Per Strand and Andrew Cooke, Osteras, Norway, pp.135-138. MAFF (1994). Radioactivity in surface and coastal waters of the British Isles. Aquatic Environment Monitoring Report. Ministry of Agriculture, Fisheries and Food, Lowestoft, UK. MAFF (1996). Radioactivity in food and the environment, 1995. Ministry of Agriculture, Fisheries and Food, Lowestoft, UK. Mashkovich, V.P. (1982). Protection from Ionizing Radiation. Moscow, Energoatomizdat (in Russian). Sazykina, T.G., Kryshev, I.I. and Kryshev, A.I. (1998). Doses to marine biota from radioactive waste dumping in the fjords of Novaya Zemlya//Radiation Protection Dosimetry. Vol.75, No.1-4, pp.253-256. Sjoeblom, K.-L. & G.S.Linsley, G.S. International Arctic Seas Assessment Project (IASAP). In: Environmental Radioactivity in the Arctic. Eds.:Per Strand and Andrew Cooke, Osteras, Norway, pp.15-20, (1995). UNSCEAR (1996).Effects of radiation on the environment. United Nations Scientific Committee on the Effects of Atomic Radiation, Report to the General assembly, Annex 1, United Nations, New York, 86pp.

7. Dose assessment for human populations

Authors : Ivan Kryshev1, Tatiana Sazykina1, A. Kryshev1, Justin Brown2, Mikhail Isopje2
1

SPA TYPHOON

Norwegian Radiation Protection Authority

7.1 TYPHOON methodology

The procedure of dose assessment, as applied to radioactive contamination of the Arctic Seas by SPA TYPHOON, comprises of the following elements: analysis of contamination sources, analysis of radionuclide migration and accumulation in the marine ecosystem, and assessment of exposure to the human population (Kryshev and Sazykina, 1993a & 1993b, 1995; Kryshev, 1995; Sazykina and Kryshev, 1997, 1998). The exposure for human was assessed in 2 parts in the present project: "actual" dose due to real levels of contamination of the Arctic Seas; and hypothetical dose associated with possible leaks of radionuclides from the radioactive waste disposal sites. Analysis of the radionuclide content in components of the marine ecosystem may be performed on the basis of observational data. The average concentrations of radionuclides in the sea water, bottom sediments and biota in 1991-1998 were collated and are presented In Chapter 3. These data were used in the calculations concerning the present radiological situation in Arctic seas. The code DOSMAN calculates annual dose to man from consumption of the Arctic seafood, based on current radioecological situation in the Arctic seas. The programme DOSMAN performs the following calculations: annual dose to a representative of average seafood consumers in the Arctic region (Barents Sea, Kara Sea); annual dose to a representative of critical group (high-rate seafood consumers); collective annual dose from consumption of seafood from a particular sea.
210

The programme is designed to calculate doses from 40K, 90Sr, 99Tc, 137Cs, The Barents and Kara seas were considered in this project.

Po,

239

Pu,

241

Am.

For average consumers, consumption rates of local seafood were chosen at a level of 30 kg/year, which is typical of the northern regions of Russia adjacent to the Arctic Seas (Consumption, 1994); consumption of other seafood is not included in the traditional diet. The diet for high-rate seafood consumers (Natives of the Russian North) is assumed to be the following (kg y-1): fish 220; mollusks 2; crustaceans 3; sea mammals 5. Calculations of individual doses (Sv/y) are made using the formula:
i Dind = ( RATION j C ij ) DFint ; i j

7.1

where : RATIONj - is annual consumption of the j-th type of seafood; Cji activity of i-th radionuclide in j-th type of seafood;

DFinti-dose conversion factor for intake of the i-th radionuclide; Collective doses are calculated based on average catches of seafood in each sea (Barents and Kara Seas). Since the catches of marine products vary from year to year, the average catches for the period 1985-1992 were estimated. For statistical calculations the Barents Sea was considered as ICES subarea I, including Spitsbergen and Bear Island area (ICES subarea IIb). Fishery data were taken from ICES fishery bulletins,as well as from Russian and Norwegian fishery yearbooks (Fishery, 1990-1995; ICES, 1988-1992; Ressursoversikt, 1995; Russia, 1988-1993). Rounded annual catches of marine products in the Barents Sea were estimated at the following levels (tonnes/year) (Sazykina & Kryshev, 1997): fish, 660,000400,000; crustaceans, 70,00030,000; molluscs, 20,00015,000; seaweeds (d.w.), 4,3003,400 (Russian catch only); marine mammals, 750-780 (catch in 1993); For the dose assessment, it was assumed that 50% of the fish annual catch, 30% of crustaceans, 30% of sea mammals, 15% of molluscs and 10% of seaweed are consumed directly by the world population. Calculations of annual collective doses (manSv y-1) are made using the following formula: Dcoll = ( CATCH j C ij FR j ) DF ji ; where : CATCHj is the annual catch of j-th seafood in a given sea; Cji activity of i-th radionuclide in j-th type of seafood; FRj- fraction of catch directly consumed by humans; Within the framework of the International Arctic Seas Assessment Project (IASAP), the Source Term Working Group has developed several scenarios for the potential radionuclide release patterns from the spent nuclear fuel of sunken submarine reactors and activated components within the reactors (Lynn et al., 1995). Radioactive waste disposals in the Abrosimov Bay, Tsivolki Bay, Techenija Bay and in the Novaya Zemlya Trough were taken into consideration as the sources of radioactive releases. 7.2

7.2 NRPA methodology

One of the general assumptions for box modelling of the dispersion of radionuclides in marine system relates to instantaneous mixing in each box which, in term, results in practical calculations to an instantaneous mixing in the whole of oceanic space. A new approach for box modelling, which includes dispersion of radionuclides during time, was therefore created in order to provide a better and more realistic/physical approach comparing to traditional box modelling. Calculations of concentrations of radionuclides in the marine environment and doses for man for some scenarios indicate differences of up to orders of magnitude between the traditional and new approach for box modelling. The present model is an improved version of the compartmental model (Nielsen et al., 1997). The equations of the transfer of radionuclides between the boxes are of the form:

n n dAi = k ji A j k ij Ai ( t T j ) k i Ai + Qi , t Ti dt j =1 j =1

7.3 Ai = 0, t < Ti Where : where kii=0 for all i, Ai and Aj are activities (Bq) at time t in boxes i and j; kij and kji are rates of transfer (y-1) between boxes i and j; ki is an effective rate of transfer of activity (y-1) from box i taking into account loss of material from the compartment without transfer to another, for example radioactive decay; Qi is a source of input into box i (Bq y-1); n is the number of boxes in the system. Ti is the time of ability for box i (the first times when box i is open for dispersion of radionuclides) and is an unit function:

1, t Ti ( t Ti ) = 0 , t < Ti .
The times of ability Ti

Ti =

m ( v 0 , vi ) M i

min

w
j ,k

jk

are calculated as a minimized sum of the weights for all paths (v0,...,vi) from the initial m box (v0) with discharge of radionuclides to the box i on the oriented graph G=(V, E) with a set V of nodes vj correspondent to boxes and a set E of arcs ejk correspondent to the transfer possibility between the boxes j and k. Every arc ejk has a weight wjk which is defined as the time required before the transfer of radionuclides from box j to box k can begin (without any way through other boxes). Weight, wjk, is considered as a discrete function F of the water fluxes fjk, fkj between boxes j and k, geographical information gjk and expert evaluation Xjk. Mi is a set of feasible paths from the initial box (v0) to the box i (vi). It is interesting to note that traditional box modelling is a particular case of the present approach when all times of ability are zero: { Ti } = 0, i = 1,..., n. Furthermore, it is significant to note that the uncertainty of calculations does not increase in comparison to traditional modelling, because graph G=(V, E) is constructed from the same information which is used for traditional box modelling. This means that the developed approach does not incorporate new, additional parameters, but utilises initial information as far as possible The new approach has been developed under the Polar institutes Transport Programme. Further details can be found in that report and elsewhere (Isopje et al., in press).

7.3 Human doses derived from archived data

7.3.1 Individual doses
Individual dose rates to average consumers, eating seafood from the Barents Sea, were (in the 1990s) approximately 2.4 x 10-7 Sv/year. Current dose rates to average consumers, eating seafood from the Kara Sea (in the 1990s), were approximately 5.7 x 10-7 Sv/year. An estimation of the maximum individual dose rates was made for a hypothetical critical group of fishermen,

consuming extremely high amounts of seafood (CEC, 1990). Individual dose rates to high-rate consumers, eating seafood from the Barents Sea, are estimated at 2.8 x 10-6 Sv/year. High-rate consumers, eating fish from the Kara Sea, receive an annual dose of about 4.2 x 10-6 Sv/year. According to these assessments, the levels of technogenic radiation risk from Arctic seafood consumption is very small (10-8-10-7).

7.3.2 Collective doses

The current collective dose rates to the world population associated with consumption of Arctic seafood were estimated, using averaged data on catches of seafood and its contamination. The consumption of seafood harvested in the Barents Sea forms dose rates to the world population of about 2.7-4.5 manSv/year (for the years with the average and maximal harvest of seafood), see Table 7.1. The contributions of different seafood items to dose are as follows: fish - 92.6%; crustaceans - 4%; seaweeds - 1.7%; molluscs- 1.4%; sea mammals-about 0.3%. The contribution of 137Cs to the annual collective dose is about 90%, 90Sr and 239,240Pu - 5% each. The current collective dose rate from consumption of seafood harvested in the Kara Sea is estimated at about 0.03 manSv/year and can be considered insignificant.
Table 7.1. Current annual collective doses to the world population from consumption of seafood harvested in the Barents and Kara Sea

Seafood item

Dose, manSv/year

Share 137 Cs,% 93.7% 51 % 61.8% 24% 96.4% 90 %

of

Share of 90Sr, % 3.3 % 3% 5.3 % 52 % 2.2 % 5%

Share 239,240 Pu,% 3% 46 % 32.9 % 24 % 1.4 % 5%

of

Fish 2.5-4.2 Molluscs 0.04-0.07 Crustaceans 0.11-0.16 Seaweeds 0.05-0.08 Sea mammals* 8.5 x 10-3 TOTAL 2.7-4.5 * Preliminary estimates

7.4 Human doses derived from release scenarios TYPHOON

7.4.1 Assessment of the long-term radiological consequences of RW dumping in the Arctic Seas - TYPHOON
Within the framework of the International Arctic Seas Assessment Project (IASAP), the Source Term Working Group has developed several scenarios for the potential radionuclide release patterns from the spent nuclear fuel of sunked submarine reactors and activated components within the reactors (Lynn et al., 1995). Radioactive waste disposals in the Abrosimov Bay, Tsivolki Bay, Techenija Bay and in the Novaya Zemlya Trough were taken into consideration as the sources of radioactive releases. For all of the scenarios, the predicted collective doses are very small and are less than 0.13 man-Sv. The individual dose rates predicted on the scenarios are (0.3-1.2)*10-7 Sv/year (Sazykina & Kryshev, 1997).

7.4.2 Assessment of the long-term radiological consequences for various discharge scenarios - NRPA

1.4 1.2 1.0 0.8 0.6 0.4 0.2 0.0 0 10 20 30 40 50

C (manSv / manSv)

Dose to man, present model C= -------------------------------------------Dose to man, Nielsen et al., 1997

1 2 3 4 5 6

Year

Figure 7.1. Comparison of doses calculated by present approach and traditional modelling.

1 and 2 - discharges of 137Cs into Novaya Zemlya Bay and into Barents Sea, correspondently; 3 - discharge of 239Pu into Barents Sea, 4 - discharge of 90Sr into Cumbrian Waters; 5 and 6 -discharge of 60Co into Obskaya Guba without and with account to the fishery in this area.
A ratio of doses calculated by the present approach and traditional modelling for 1 TBq

discharges of different radionuclides and scenarios are shown in Figure 7.1. Plots indicate that, for some radionuclides and scenarios the differences between the results of dose calculations could be up to orders of magnitude in the initial phase of dispersion in comparison with traditional modelling. It is of interest that a ratio of doses calculated is subject to wide variations for different radionuclides, scenarios and time. Further details can be found in the Polar Institutes Transport programme report and elsewhere (Isopje et al., in press).

References
CEC (1990). The radiological exposure of the population of the European community from radioactivity in North European marine waters. Project Marina, Commission of the European Communities. Bruxelles: EUR 12483. Iosjpe, M., Brown, J. & Strand, P. (in press). One Approach for Box Modelling of Radiological Consequences from Releases into Marine Environment. Journal of Environmental Radioactivity. Kryshev, I.I. (1995). Reconstruction and prediction of radioactive contamination of the ecosystems of the Arctic Seas//Environmental Radioactivity in the Arctic. Edited by Per Strand and Andrew Cooke. - Osteras, Norwegian Radiation Protection Auuthority, p.238-240. Kryshev, I.I. and Sazykina, T.G. (1993a). Dynamic model for assessment of radioecological situation in Arctic Seas. Dose and risk assessment. In: International Meeting on Assessment of Actual and Potential Consequences of Dumping of Radioactive Waste into Arctic Seas. Working Material. Oslo, February 1-5, 1993. Vienna, IAEA. Kryshev, I.I. and Sazykina T.G. (1993b). Estimated ecological risk due to radioactive contamination of the Kara and Barents Seas. In: Izvestia visshikh uchebnikh zavedeniy. Yadernaya energetica. No.2, 81-89 ( in Russian). Kryshev, I.I. and Sazykina, T.G. (1995). Radiological Consequences of Radioactive Contamination of the Kara and Barents Seas. J. of Environmental Radioactivity, Vol.29, N 3, p.213-223. Lynn, N., Timms, S., Warden, J. et al. (1995) Scenarios for Potential Radionuclide Release from Marine Reactors Dumped in the Kara Sea. In: Environmental Radioactivity in the Arctic. Eds.:Per Strand and Andrew Cooke, Osteras, Norway, pp.135-138. Nielsen S.P., Iosjpe M. & Strand P. (1997). Collective doses to man from dumping of radioactive waste in the Arctic Seas. The Science of the Total Environment, 202, 135-146. Sazykina, T.G. & Kryshev, I.I. (1997). Current ant potential doses from Arctic seafood consumption//The Science of the Total Environment, 202, pp.57-65. Sazykina, T.G., Kryshev, I.I. and Kryshev, A.I. (1998). Doses to marine biota from radioactive waste dumping in the fjords of Novaya Zemlya//Radiation Protection Dosimetry. Vol.75, No.1-4, pp.253-256.

8. Development of guidelines for vulnerability assessment

Authors : Justin Brown, Mikhail Iospje & Anne Liv Rudjord Norwegian Radiation Protection Authority

8.1 Introduction
The following text is partly based on the work of the radioecological sensitivity forum (CEH, 2000) with additional interpretations and views of the authors of this chapter. Such a strategy was adopted because of the clear requirement to maintain an internationally-recognised approach in the development of vulnerability assessment guidelines. The first key point to note is the fact that the term vulnerability has been used in other disciplines and contexts and may therefore cause misunderstanding. Vulnerability for example has been used to describe how severe the likely consequences of system failure may be. This definition is useable in the present context if the words system failure are replaced by radioactive pollutant loading however it has been widely agreed (CEH, 2000) that the less ambiguous term Radioecological sensitivity should be used. It is important to be able to readily identify major routes of exposure, the most highly exposed individuals or populations arising from radioactive contamination and the areas of most concern. Radioecological sensitivity, as a concept, addresses methods of identifying high radiation exposure, especially with regard to spatial variation in exposure. The concept can be applied to Man and other biota. Radioecological sensitivity analysis involves the integration of current knowledge on pathways. A key task is to attribute spatially the underlying processes determining transfer and thereby identify the most radioecologically sensitive areas. This identifies where high exposure may occur and why. It can consider single food products or species, or a number of highlighted key parameters to identify areas where a number of sensitive pathways occur together. Before considering in more detail what should be considered in a radioecological sensitivity analysis, it is important to make a distinction between sensitivity and risk. The concept of risk of radioactive contamination can be considered to relate to the potential for an area to suffer detriment from radioactive pollution and would therefore include components relating to, for example, proximity to nuclear installations and their safety, in addition to components relating to radioecological sensitivity. The sensitivity of the system therefore might be considered to form a sub-set of any broader risk assessment.

8.2 Considerations for a radioecological sensitivity assessment

The severity of the consequences in a marine ecosystem can be measured in terms of:

a) doses to man from intake of marine foodstuffs (fish, salt, shellfish, etc.) and from external radiation due to recreational or working activities (e.g. sailing, bathing, fishing). b) economy, including production reduction and quality deterioration (in relation to limits set by regulatory authorities), as well as intangible effects such as loss of image (e.g. recreational areas). c) ecological impact (e.g. reducing biodiversity, mutations, imbalance of foodchains). Any assessment of radioecological sensitivity requires firstly a clear definition of the terminology and secondly a methodology for quantifying the terminology. In order to facilitate the task of defining radioecological sensitivity, a useful exercise involves dividing the marine ecosystem into component parts under the broad abiotic and biotic headings. In this way the parameters that influence the transport and fate of radionuclides in marine ecosystems can be identified and the potential importance of these parameters in causing the consequences/effects listed above ((a) to (c)) can be qualified.

8.2.1 Abiotic
8.2.1.1 Seawater The chemical composition of the major components (Na+, K+, Mg2+, Ca2+, Sr2+, Cl, SO42-, HCO3- etc.) of seawater in the worlds oceans and seas generally varies to a small extent. However, in certain environments including estuaries, anoxic basins and hydrothermal vents, the major composition of seawater can change significantly (Millero, 1996). The evaluation of the direct effect this may have on concentrations of radionuclides is problematic although variations in Kd for some radionuclides may be observable possibly resulting from exchange reactions with competitive ions. The Kd for 137Cs, for example, is often higher in freshwater aquatic environments (Meili, 1994, Comans et al., 1989) than for marine environments (IAEA, 1985) although the processes responsible for this observation may be numerous. The minor elements found in seawater have concentrations that are more dramatically influenced by inorganic and biological reactions and therefore exhibit a wider range of concentrations. The group includes the biolimited elements P, N and Si. In the case of P, for example, total concentrations and partitioning between inorganic and organic fractions may vary significantly on small spatial and short temporal scales owing to phytoplankton blooms and up-welling (Millero, 1996). Certain radionuclides behave as chemical analogues for minor elements with the result that the mapping of stable minor element distributions could give valuable insight into the behaviour and fate of these radionuclides. Other chemical parameters, in particular Eh and pH can strongly influence the behaviour of certain radionuclides. When considering the mobility of Pu in aquatic systems, for example, the distribution coefficient is known to be oxidation-state and thus Eh dependent, with Pu (III, IV) generally exhibiting higher Kds than Pu (V, VI) (Nelson & Lovett, 1978). Physical parameters also influence the behaviour of radionuclides. For a defined volume of water, for example, the % of a radionuclide associated with suspended particulates will be correlated with the suspended load. Sholkovitz (1983) has expressed this as a simple model in the context of Pu behaviour. Applying the model to measured suspended loads and Kd values, one discovers that at the suspended loads observed in the pelagic oceans, Pu (oxidized and reduced) should exist in the dissolved phase whereas for high suspended load areas, such as

those observed in coastal environments and estuaries, Pu is primarily associated with suspended particles. It may, therefore, be necessary to map areas of selected seas and oceans where major and minor seawater composition and/or selected chemical and physical parameters differ significantly from normal values. Clearly, this is no simple task when one considers the dynamic nature of some marine systems. Simplifications, e.g. annual averaging may be required in numerous situations. Following the mapping work, the behaviour of selected radionuclides in these environments could be considered, possibly in terms of whether the area is acting as a potential source or long-term sink of each radionuclide. Simplistically expressed, those areas that, through processes related to water chemistry variations, accumulate radionuclides will be areas where doses to man and biota and economic impact will be highest. It has been suggested (CEH, 2000) that historical records of radionuclide activity concentrations in marine ecosystems could be used to determine the coastal areas where maximum and minimum fallout occurred (its spatial variability). This can contribute to identify areas that are more susceptible to radionuclide accumulation following inputs from atmospheric fallout. 8.2.1.2 Sediments For local-scale contamination by long-lived radionuclides, the inverse relationship between grain-size and activity concentration of particle-reactive radionuclides is well established. For example, numerous studies (e.g. Hetherington and Jeffries, 1974; Assinder et al., 1993, Mudge et al., 1994) have reported a close correlation between the activity concentrations of Sellafield-derived radionuclides, including 137Cs239,240Pu, and 241Am, and fine-grained sediments, e.g. silts and clays, in the marine and estuarine deposits of the Irish Sea. Areas in the marine environment where fine-grained sediments exist are therefore likely to be sensitive to the accumulation of radionuclides. The organic content of sediments is also known to be important in the context of the behaviour of some radionuclides. Studies in the Irish Sea have shown that the geochemical phase association of Pu isotopes with organic complexes is significant (Brown et al., 1997). Areas of organic-rich sediments could therefore be identified as potential sites of Pu accumulation. Sedimentation and diagenetic processes including sedimentation rate, bioturbation and redox controlled reactions may strongly influence the behaviour and fate of radionuclides in marine environments. Some of these parameters may vary significantly over regional spatial scales. Sedimentation rates, for example, can vary from a low rate of 1mm per 1000 years in deep oceanic basins to the dynamic erosional-accumulative cycles often observed in estuaries where annual accumulation rates can exceed centimetres per year. Areas of high sediment deposition may form significant sinks for long-lived particle-reactive radionuclides although the deep burial of highly contaminated sediment (assuming a pulsed contamination input) by cleaner sediments may offset the impact to man owing to the fact that people would be shielded from elevated external radiation exposures. It should be noted that whether we are concerned with situations in which radionuclides are deposited from the atmosphere (as occurs during global fallout) or with a situation in which

radionuclides are discharged to a coastal environment (as occurs during the operation of nuclear reprocessing plants) we are primarily concerned with processes initially occurring in marine surface waters. (An exception to this is the marine dumping of radioactive material). The sediments that are immediately affected will be those deposited in coastal environments. Sediments forming the major fraction of oceanic basins are unlikely to be affected on short time scales. Transfer of radionuclides to the sediments of deep ocean basins (up to several km is depth) can occur by processes including radionuclide uptake and excretion by biota and downward transport of faecal particles (time scale of months to years) or by the advection of water masses containing dissolved radionucldes into oceanic basins followed by direct interaction and adsorption of radionuclides onto sediment surface (a process that is likely to occur over much longer time-scales). It immediately becomes apparent that sediments in coastal or shallow marine environment are more vulnerable to contamination from short-lived radionuclides. The bathymetry may also be a consideration in assessing the sensitivity of a marine area. An approach to the assessment of radiological sensitivity of marine environments may involve the mapping of sediment types. Depending on the criteria used in the assessment of radiological sensitivity, simple models could be applied where sedimentological parameters are mapped onto selected end-points.

8.2.2 Biotic
8.2.2.1 Flora and fauna The biological productivity of different sea areas varies widely. The Arctic Ocean basin, for example supports marine biological communities that are comparable, although reduced in abundance and complexity to those in northern temperate oceans (Murray, 1998). The level of phytoplankton primary production tends to be relatively low (~10 g C/m2/y) in central Arctic Ocean Regions whereas in continental shelf areas, such as the Barents Sea, rates of primary production can be much higher (> 100 g C/m 2/y) (Murray, 1998). Ice edges and associated water column features are key areas of elevated productivity in the Arctic. In the context of the criteria (Section 8.2 (a) to (c)) for radieological sensitivity analyses cited above, it becomes apparent that those areas with high biological productivity will be sensitive in the sense that they are areas where (i) a relatively large biomass could be exposed to internal and external radiation sources, (ii) fluxes of radioactivity to man could be significant and (iii) the economic impact could be high. The latter 2 points are dependent on whether a particular component of the biomass (food-chain) is harvested for human consumption. It should be noted that mapping biological productivity, or components thereof, is no simple task. In the first case there is a clear influence of depth on the concentration of primary producers phytoplankton etc. will be mainly found near the surface of the water column where light energy sources are at a maximum. A 2-dimensional representation of productivity may therefore be insufficient. Secondly, large seasonal variations in light and nutrient inputs, especially in the Arctic, result in large temporal variations in biological productivity. Significant time-averaging may be required in order to reduce any mapping task to manageable proportions. The species characterising a selected marine area may also influence our evaluation of the sensitivity of that area. For example, an area heavily populated by sea mammals might be considered sensitive by virtue of the fact that the radiosensitivity of mammals from

exposure to ionising radiation is relatively high compared to the majority of other taxonomic groups (UNSCEAR, 1996). In another example, where the criteria for assessment are doses to man or economical detriment, areas where populations of stocks of harvestable fish species are present might be classified as sensitive. Once again the mapping of areas in terms of key or selected species is no easy task especially when one considers the migratory nature of many marine fauna. 8.2.2.2 Man Committed effective dose equivalents and/or collective doses, clearly provide another route into a radioecological sensitivity assessment. External doses are likely to be of minor concern owing to the fact that (i) the bulk of contaminated sediments will be overlain by water effectively shielding an individual from exposure and (ii) exposure from contaminated water is unlikely to be high because humans do not inhabit the marine environment. Of course, external irradiation is possible in some areas e.g. inter-tidal and coastal areas used for recreational activities. Such areas might immediately be considered sensitive in the context of external irradiation exposure. With respect to internal doses, marine environments from which resources are collected for human consumption could be defined as sensitive. In other words, sensitive areas might be those that would contribute to a relatively high internal dose to man, via marine transfer pathways, for a given input of radionuclides. At a simple level, collective doses may be calculated using predicted activity concentrations, production statistics and collective dose conversion factors in order to allow comparison between marine areas. In order to consider the dose distribution or doses to individuals or critical groups of individuals, however, dietary information would be required which can vary significantly. For selected fishing/harvesting grounds an analysis of the destination of the marine products may be required with the goal of establishing whether the products are mainly consumed by a small critical group, or whether the products are exported and consumed in smaller portions by a large diffuse group.

8.3 What can be practically included in a radioecological sensitivity assessment ?

In the section above it is clear that a number of parameters might be considered in the process of conducting a radioecological sensitivity assessment. Below one possible approach is outlined, based on the recommendations of CEH (2000). Intuitively, Radioecological sensitivity has to do with the detriment, injury or ill effects induced by an event. Given the historical bias of the ICRP and radiological sciences towards the protection of man, Radioecological sensitivity may be defined as the expected ultimate detriment to man from a given radioecological disturbance. This definition forms a useful starting point but one should bear in mind that a broader definition may be required once criteria and methodologies relating to the protection of the environment from ionising radiation have been developed. Given this definition, one has to decide which already defined physical quantity best expresses the notion of detriment.

8.3.1 A scenario for the quantification of Radioecological Sensitivity

Let us consider a region of area A (m2) which receives a total deposition P (Bq) of some radionuclide I (137Cs, 90Sr, etc.). According to an initial scenario we may consider as the detriment to a person living in this region the effective dose that he will receive from this deposition until he or she reaches a predefined age T0 (e.g. T0 = 70 y). This scenario is explored in some detail below. 8.3.1.1 Specific Radioecological Sensitivity The effective dose that an individual receives over a period of time, until they reach the age of T0 years, depends both on the isotope I that causes the dose and the age of the individual T at the time of onset of the deposition. Subtracting all factors of geometry (the area of the region, the intensity of the deposition and the composition of the population) we may define a basic specific physical quantity, which we may call Partial Radioecological sensitivity SI(T) as The effective dose, accumulated by an individual of age T at the time of the incident until he or she reaches the age T0, if the deposition of isotope I in the region is 1 Bq m-2. If one accepts this definition, then the concept of Radioecological sensitivity of a region is best represented by the average effect of the exposure to the deposition of all ages represented in the population. Thus, the Radioecological sensitivity of a region to isotope I can be defined as SI =

T0 0

S I (T ) f (T ) dT

(8.1)

in which f(T) is the age distribution function of the population, normalised to unity, i.e.

T0 0

f (T ) dT = 1 .

(8.2)

For a mixture of isotopes in the deposition one can go one step further and define a quantity that describes the Radioecological Sensitivity of a region with a single number. If aI is the fractional population of isotope I in the deposition, one can introduce the quantity S=

a
I I

SI

(8.3)

with the condition, for normalisation purposes,

a
I

= 1.

(8.4)

All physical quantities introduced above as some form of Radioecological sensitivity are measured in Sv Bq-1 m2. 8.3.1.2 Integral Quantities The integral physical quantity that emerges naturally in this scenario is what can be

provisionally termed the Expected Detriment (due to a specific isotope I) DI. Again, intuitively, the Expected Detriment to a region should be: proportional to the Radioecological sensitivity SI of the region proportional to the deposition PI of isotope I in the region proportional to the population N affected inversely proportional to the area A of the affected region. Folding in the geometry of the region we may thus write DI = PNS I = pNS I A (8.5)

where in the last step of eqn (8.5) we have used the specific deposition p (Bq m-2) in the region p= P . A (8.6)

Finally, following the practice reflected in eqn (8.3) one can define the Detriment to a region due to all isotopes in the deposition, expressed with a single number, through the relation
D=

a D
I I

(8.7)

under the normalisation condition of eqn (8.4). The units of the Expected Detriment DI and the Expected (Grand, Total) Detriment D are man Sv.

8.4 Calculation of Radioecological sensitivity

The quantity that needs to be calculated first according to the above scenario is the Partial Radioecological sensitivity SI(T). The steps in the calculation proposed by this scheme are as follows: 1. The dietary habits of the population in the region are determined and food products of primary importance in the diet (e.g. fish, mussels) are identified. A model diet for the region is determined in the form of a set of coefficients {bm}, each of which represents the daily, monthly or yearly intake of food product m (e.g., in kg d-1). 2. By definition, the aggregate transfer coefficients Tag(I,m) for the transfer of isotope I to food product m in the model diet is the contamination concentration in the product resulting from a deposition of 1 Bq m-2. Thus the total activity intake R(I) of an individual in the region, resulting from a deposition of 1 Bq m-2 of isotope I, will be given by R ( I ) = Tag ( I , m) bm
m

(8.8)

where the sum extends over all items in the model diet. 3. Given the daily intake R(I), the Partial Radioecological sensitivity SI(T) may be calculated by converting from activity intake to committed effective dose using relevant conversion factors (e.g. Phipps et al., 1991). Following this calculation, one could proceed to calculate the quantity in eqn (8.1), which

further requires knowledge of the age distribution function f(T). It is noted that the shape of f(T) will significantly affect the radioecological sensitivity of a region. Since activity intake is expected to affect younger age-groups to a much greater degree, a skewed age distribution curve, such as that encountered in many villages in the contaminated regions near Chernobyl (where only old people remain in the village) will result in a lower numerical value of SI.

8.5 Recent developments made, with respect to radiecological sensitivity analysis, within the Effects Programme
For the purpose of evaluating radiological sensitivity, one of the main tasks is to model the sensitivity index for parameters that characterise the environment (area, volume, etc.). This problem can be illustrated by modelling the radiological sensitivity of marine areas by the NRPA box model for radiological assessment of Arctic Ocean and adjacent seas. The index D(i)/A(i) was used (here D(i) is a collective dose to man from the box i and A(i) is area of surface waters for the box i) following an input of 10 kBq m-2 137Cs (Figure 8.1).

Figure 8.1. Collective doses to man per area (manSv/m2) from different marine areas (boxes) after 137 Cs uniform deposition 10 kBq/m2.

The other possibility to evaluate radiological sensitivity of marine regions is to calculate the load of radionuclide for each region (box) that will lead to the limit of allowable concentration of radionuclide in sea products, for example, fish. This case is illustrated in Figure 8.2.

Figure 8.2. Uniform deposition of 137Cs per area (kBq/m2) which will lead to concentration of radionuclide 600 Bq/kg in fish one year after input.

Both approaches give similar information (a high flux roughly corresponds to a low action load), in essence the shallow coastal areas and shelf seas, e.g. North Sea, Baltic Sea, Skagerrak and Kattegat are the most vulnerable to deposition of radiocaesium. In these particular approaches, the depth of the water column and the magnitude of the seafood catch in each box would appear to be the parameters driving the degree of vulnerability. It should be stressed that the assessment of vulnerability in the marine environment is at a preliminary stage and will require further development of concepts and models before a welldefined and robust methodology is in place.

8.6 Recommendations for future monitoring programmes

A monitoring programme for radionuclides in the northern marine environment must be designed to consider both actual and potential sources of radioactive contamination, and the potential impact of these sources on human health, the environment and also on the exploitation of marine resources (mainly fishing industry). A main objective will clearly be to document the activity concentrations of radionuclides in commercially important fish species for the purpose of demonstrating compliance with food safety standards and instilling consumer confidence. Although the activity level of many radionuclides in northern marine waters are relatively low, the fact that discharge regimes from nuclear facilities can change significantly over time or accidents can occur which lead to widespread contamination in the marine environment precipitates the need for a comprehensive and frequent sampling programme. A recent case in point can be given by the increasing levels of 99Tc in biota that have been determined in Norwegian coastal waters in the late 1990s following increased releases of this radionuclide to the Irish Sea from BNFL Sellafield. The many potential sources of radioactive contamination, including dumped radioactive waste, sunken submarines and all the nuclear installations in north-west Russia means that the programme must also supply information that will be applicable to a potential accident or in a situation where increased releases are occurring.

8.6.1 Monitoring areas

In relation to present day contamination, most anthropogenic radionuclides arising in western European marine environments are transported to the Barents Sea through the Norwegian Coastal Current. Consequently monitoring stations should include coastal stations in northern Norway and Russia, and in the open Barents Sea including the important fishing areas. In addition, in order to detect potential future releases, sampling and/or continuous monitoring should be carried out close to the potential sources that exist in this area, for instance the recently sunken submarine Kursk and dumped radioactive waste in the Kara Sea. Also the discharges from the large Russian rivers Ob and Yenisey may be regarded as both existing and potential future sources of radionuclides. Monitoring routes following the prevailing marine and ice transport pathways through the Arctic should be considered. Furthermore, a monitoring programme should preferentially supply data that allows the longterm transport and behaviour of radionuclides to be predicted. Such information is an important requirement of consequence assessment models. Therefore, a sampling programme for this purpose should also be defined. Finally, high levels of contamination exist on a localised scale in a number of bays in Novaya Zemlya. Monitoring these areas should also be carried out with the purpose of detecting longterm changes and possibly radiation effects on biota in situations where the environment is highly contaminated.

8.6.2 Sampling programmes

Conventionally, monitoring programmes include simultaneous sampling of water, sediment and biota, which should clearly also be performed here. Such an approach provides a good overview of the environmental contamination and the chance to extract refined and site specific parameter values that can benefit consequence assessment models. On the basis of the present project results and on the international work presently carried out concerning protection of species other than man for harmful effects of radiation, special emphasis should be put on the sampling of biota. The activity concentrations of radionuclides are essential in the evaluation of radiation doses to both humans and other living species. For humans, a dominating exposure pathway will be consumption of marine foodstuffs. As shown in Chapter 7.3.2, the collective doses from fish consumption dominates today, but different contamination scenarios, resource situation and eating habits may change this conclusion in future or longer time-scale assessments. For the purpose of monitoring doses to humans, sampling should include fish, crustaceans, molluscs, seaweeds and possibly sea mammals that are the most relevant for human consumption today, or which have the potential to become important in the future. Measurements should be performed on the edible fractions of the biota samples. A new framework for protection of biota from adverse effects of radiation is expected to emerge within the next few years; therefore, a future monitoring programme must be designed accordingly. Information on activity concentrations in whole body/muscle of organisms are suitable for dose calculation in line with current monitoring practice but more detailed information may be required, whereby selected organs within the organisms are analysed to allow more robust whole body dose rates to be determined. The relationship between radiation dose and possible effects is a subject of further research. A suitable approach may be the identification of suitable reference organisms that can be selected to represent the larger ecosystem. Any future monitoring work will need to integrate the recommendations made by ongoing research projects that aim to identify such biota types in the marine environment. In addition, the compilation of data pertaining to dose effects relationships for selected reference species may be required. The types of effects that may be studied cover a range of dose rates and endpoints, from sub-cellular cytogenetic damage at relatively low dose-rates through to effects on the reproductive success of organisms, i.e. effects on fertility and fecundity, and finally, in high radiation level environments (such as those that may be present near to dumped nuclear objects), to lethal effects. An integrated approach including all the abovementioned components will allow a transparent monitoring and assessment to be made of the environmental impact of radioactivity.

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