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US Particulate and Xenon Measurements Made Following the Fukushima Reactor Accident

INGE 2011 Yogyakarta Workshop, Justin McIntyre1, Steve Biegalski2, Ted Bowyer1, Matt Copper1, Paul Eslinger1, Jim Hayes1, Derek Haas1, Harry Miley1, J.P. Rishel1, Vincent Woods1

1 2

Pacific Northwest National Laboratory, Richland, Washington, USA The University of Texas at Austin, Austin, Texas, USA

Views expressed here do not necessarily reflect the opinion of the United States Government, the United States Department of Energy, or the Pacific Northwest National Laboratory

Outline
Event Network Atmospheric Transport Detections Isotopic Ratios Conclusions
Material in this presentation is covered in more depth in the following journal submissions.
S. Biegalski, et al., US Particulate and Xenon Measurements Made Following the Fukushima Reactor Accident, accepted for publication in Jour. of Envir Radioactivity, 2011 T. Bowyer, et al., Elevated Radioxenon Detected Remotely Following the Fukushima Nuclear Accident. Jour. of Envir. Radioactivity 102 (7):681-687. doi:10.1016/j.jenvrad.2011.04.009 P. Eslinger, et al., Source Term Estimation of Radioxenon Released from the Fukushima Daiichi Nuclear Reactors Using Measured Air Concentrations and Atmospheric Transport Modeling, to be submitted in Jour. of Envir. Radioactivity, 2011

Event
The March 11, 2011 9.0 magnitude undersea megathrust earthquake off the coast of Japan and subsequent tsunami waves triggered a major nuclear event at the Fukushima Daiichi nuclear power station. At the time of the event, units 1, 2, and 3 were operating and units 4, 5, and 6 were in a shutdown condition for maintenance.

Boiling Water Reactor

Unit Fukushima Daiichi 1 Fukushima Daiichi 2 Fukushima Daiichi 3

Design BWR-3 BWR-4 BWR-4

Containment Mark I Mark I Mark I

Electric Power 460 MW 784 MW 784 MW

Thermal Power 1,380 MW 2,352 MW 2,352 MW

Following Radioactive Release Timeline Fukushima the Fukushima Detection


Evidence of radionuclide released reached the Japanese IMS station within 2-3 days First evidence of the plume hitting the United States came to PNNLs experimental equipment about 1 day later (March 16)

US Radionuclide Stations + Richland, WA

Salchaket, AK Sand Point, AK Richland, WA Sacramento, CA

Ashland, KS Charlottesville, VA Melbourne, FL Midway Islands Wake Island Upi, Guam

Oahu, HI

Palmer Station

First detection of radioxenon in US at Richland WA Our First Results


Xenon-133 measurements were x450,000 our detection levels using a SAUNA-II xenon measurement system Noble gas does not washout, and is the first emitted from any possible fuel damage Levels persisted for weeks and isotopes were ultimately detected across the northern hemisphere and around the world

U.S. IMS Station Detections


U.S. stations detected both particulate and noble gas emitted from the event. Initial 133Xe detections in Richland, WA (non-IMS station) were on March 16, 2011. Several volatile radio-isotopes were detected
Missing were several isotopes that were highly indicative of a nuclear explosion

131I

Activity Concentration

131I

Activity Concentration

133Xe

Activity Concentration

Isotopic Ratios
SCALE6/ORIGEN-ARP models were conducted to model predicted isotopic ratios (same models used for inventory calculations). Comparisons were made between model and measurements. Good comparison adds validity to models and to measurements. Shows that all stations are measuring the same event.

133I/131I

Activity Ratios

(Indicative of gaseous releases)

134Cs/137Cs

isotopic activity ratio

136Cs/137Cs

isotopic activity ratio

133Xe/131mXe

isotopic activity ratio


HEU Pulse

Aerosol Network Take AwayLessons Learned Aerosol Observations/ Points


Network worked as planned
Event was equivalent to a 20kT above-ground nuclear explosion Indicates network is capable across at least 5 orders of magnitude for measured concentrations Sampling sites were able to report fission products without being overwhelmed, site closest to accident had trouble because of extremely high activity and power outages. Radionuclide concentration analysis clearly indicated that this was a reactor accident/release. Isotopes measured are consistent with a nuclear reactor Lack of short-lived refractory isotopes indicative of a reactor Nearby stations had significant increases in MDCs caused by this event, however ATM allowed predictive plume hits and impact to down wind stations. Not all of the network was affected all of the time Need additional analysis to determine how impacted nearby stations were and would they still be able to detect a 1kT above ground test
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Aerosol Observations/ Lessons Aerosol Network Take Away Points (2) Potential improvements

Learned

Initial RASA measurements were possible before the filter was measured Detector may need additional shielding from environmental influences Intermittent power loss was significant at RN-38 Improved mechanisms for recovery from power loss Takes ~3 days to get sample counted and reported Need first look early response systems with real time measurements (e.g., NaI, CsI) for high activity events Suggest the need for a emergency situation software script or state to reduce per-sample activity (sample for 6, 12, or 24 hours) Potential to incorporate future accident measurements into existing radiological safety protocols (discussed at ISS-11) Not unlike the seismic network tie in after the 2005 Tsunami Clearly outside of the original scope of the network

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Conclusions

Radioxenon Network Take Away Points


Network worked as planned
Event was equivalent to a 1Mt below-ground nuclear explosion with 1% leakage The xenon measurements made by IMS-like equipment were the highest fidelity measurements made and far superior to what was available post-Chernobyl Radionuclide analysis clearly indicates that the plume was from a nuclear reactor 2 of four radioxenon isotopes were easily detected from the Fukushima event across the globe. Xe-135 MDC was only slightly elevated by this event, providing key indicator of nuclear explosion Impacted stations are not blinded to underground nuclear explosions.

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Radioxenon Take away Lessons Gas Observations/ points (2) Learned

SAUNA dead time observed in samples with elevated count rate and was significant with very high count rates Sauna dead time corrections needed Initial high Xe levels saturated the RN-38 detector so no spectral analysis was possible Nuclear detector electronics needs to be updated to handle high count rate The MDC of the detector was highly effected from high memory effect Research and implementation on reduction of memory effect necessary (in progress). Inconsistencies with meta-stable ratios.
Need to re-analzye data sets Need better analysis methods (currently working on SDAT ). Desire >2X improvement in conversion electron resolution

Xe was first observed at Richland WA which is not part of the IMS network Need higher density of Xe systems

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Conclusions
The IMS network demonstrated that it is capable of measuring and reporting radionuclides from a single event across the globe. Measurements were significantly above the detection limits for many systems. Combination of atmospheric transport, radiation detection, and reactor modeling were fused to provide a picture of the event. Careful analysis mitigates source blinding More data analysis is required to demonstrate and further enhance second event detection.

Background slides

Initial Atmospheric Transport


Atmospheric transport models were run to predict transport of radionuclides. Models predicted that most of the radiation traveled east. First detections were in Japan, Russia, and the United States.

PNNL Aerosol Data

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137Cs

Activity Concentration

Unit 1, 2, and 3 Xe Inventories

Combining atmospheric transport, ground measurements, and inventory shows that between 85% and 103% of radioxenon inventory was released from the three reactors.

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