Radiological analysis of Namie street dust May 31, 2013 Marco Kaltofen, MS, PE Boston Chemical Data Corp.

2 Summer Street Suite 14 Natick, MA USA 01760 Department of Civil and Environmental Engineering, Worcester Polytechnic Institute Worcester, Massachusetts, USA Email: Kaltofen@wpi.edu

Abstract A sample of street dust was received from a location about 17 Km from the Fukushima-Daiichi accident site. The street is in Namie-machi, Futaba-gun, Fukushima Prefecture. This is in the restricted zone, close to, but is just outside of the exclusion zone. The dust sample was analyzed by Scanning Electron Microscopy with Energy Dispersive X-ray analysis and by sodium iodide gamma spectrometry. An autoradiograph was prepared from the sample using bluesensitive X-ray film. The sample contained 1,500 Bq/gram of combined Cs-134 + Cs-137 as well as 0.3 Bq/gram of Co-60. The sample was uniformly radioactive when analyzed by autoradiography. Analysis by SEM/EDS found widely scattered particles of suspected fission products among larger aggregates of mineral matter.

Introduction and Methods Airborne dusts can transport radioactive materials in the form of isolated individual particles containing high concentrations of radioisotopes. The specific activity of an individual particle can be significantly higher than that of the surrounding particles in a dust sample. These high activity particles, called hot particles, are isolated and analyzed by scanning electron microscopy / energydispersive X-ray analysis. (SEM/EDS). A portion of the Namie dust sample was mounted on a glass slide with conductive tape, and carbon coated and scanned by a LEO/Brucher SEM/EDS system, using a lithium drifted silicon semiconductor X-ray detector for the electron microscopy analyses. All SEM/EDS analyses were performed at Microvision Labs of Chelmsford, MA, a commercial microscopy laboratory. The electron beam current was 0.60 nAmperes, accelerated at a voltage of < 0.5 to 60 keV. Backscattered electrons are detected and provide imaging contrast determined by the atomic number of the nuclei with which it interacts. Characteristic X-rays are emitted by ions in excited states created by interaction with the electron beam. These characteristic X-rays are detected by the lithium drifted silicon detector. SEM / EDS does not distinguish between stable and unstable, (radioactive), nuclei of a given element. Additional information is required to determine whether a particle contains radioactive materials. For certain elements, including uranium, thorium, and plutonium, the known isotopes are radioactive. For other elements, including lead, yttrium and many rare earths, the known isotopes are both radioactive and stable. For elements with both stable and radioactive forms, gamma spectrometry provides confirmation of the presence of radioactive isotopes in bulk particulate samples. In this analysis, initial gamma spectrometry analyses were performed with an Amptek CdTe gamma detector and MCA, scanning the range from 10 to 2060 keV, equipped with a copper/lead multilayer shield. Laboratory-based gamma spectrometry analyses were performed with an Ortech 2 inch NaI gamma detector and lead shield.

Results and Discussion This analysis focused on fission products that are released from damaged nuclear fuels. The most common fission products found in radioactively-contaminated dusts from Fukushima Prefecture include Cs-134 and Cs-137. Nuclear reactors tend to produce both heavy (atomic weight 125 to 155) and light (atomic weight 80 to 110) byproducts. These include light radioactive isotopes of the elements yttrium and silver, plus the heavier isotopes tin, antimony, cesium, cerium, neodymium, and lanthanum. All of these were detected in this dust sample by SEM/EDS, in the form of tiny particles on the order of 10 microns in size. Examples of the SEM/EDS-detected particles in the small, (100 milligram), dust sample included thorium-containing rare particles, lead titanate, and yttrium lanthanide particles. These were in the 2 micron to 10 micron size range. The sample of street dust was also analyzed by sodium iodide gamma spectrometry. (See Figure 1) An autoradiograph was prepared from the sample. (See Figure 2) Gamma spectroscopy detected 153 Bq total of radioactive cesium, (Cs-134 + Cs-137), and uranium daughter isotopes in the 100 milligram sample. This is equivalent to 1530 Bq, per gram or 1.5 MBq per kg. Cobalt-60 was present at 0.3 Bq per gram. The most active uranium daughter isotope found by gamma spectroscopy was radium-226. (See Figure 1) The dust sample had numerous particles containing mostly lead, yttrium, various rare earths, and thorium. Some of these lead and rare earth particles were in the respirable size range, measuring only 1 or 2 microns in size. (See examples in Figures 3, 4, and 5) This dust was collected just a few hundred feet outside the exclusion zone around Fukushima-Daiichi. Occasionally observers have reported small deposits of windblown black sediment which measures higher than normal for radioactive forms of cesium and other radioisotopes. This is the first time we have examined

a sample that was clearly distinct from surrounding soils and dusts, by virtue of its high radioactivity. The sample had the highest radium-226 levels of the approximately 200 dust and soil samples analyzed by this laboratory. This analysis is a limited one, since the subject is a single (and small) dust sample. This sample is not representative of the Namie region as a whole. This data demonstrates that isolated street dusts can reach radiation levels well in excess of their general surroundings. There is not enough data in a single sample to explain why a small street dust sample was so contaminated with radioactive substances compared to surrounding materials. Clearly some environmental mechanism has allowed this more radioactive dust to remain segregated rather than dispersing into the soils or being washed away by rains. Given the resistance to dispersion of this radioactive dust, this analysis suggests that small localized radioactive hot spots can persist despite the passage of months and years since the Great Northern Japan Earthquake and subsequent radiation releases.

Author Disclosure Statement The author declares that no competing financial interests exist. The author gratefully acknowledges the efforts of Mr. Jun Ohnishi, who provided the sample for this analysis.

Following pages: Figures 1 to 5

Figure 1: Sodium Iodide gamma spectrum of Namie street dust

Figure 2: Namie dust sample X-ray film autoradiograph (right) and scaled true color scan (left).

Figure 3: Scanning Electron Micrograph w/ Robinson Detector image of a lead particle imbedded in a larger aggregate with a chart showing percent elemental composition of the particle.

Figure 4: Scanning Electron Micrograph w/ Robinson Detector image of a thorium-containing particle imbedded in a larger aggregate with a chart showing percent elemental composition of the particle.

Figure 5: Scanning Electron Micrograph w/ Robinson Detector image of a yttrium-lanthanide particle imbedded in a larger aggregate with a chart showing percent elemental composition of the particle.

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