radiological analysis of namie street dust

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    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, USAEmail: [email protected]

    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 blue-

    sensitive X-ray film. The sample contained 1,500 Bq/gram of combinedCs-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.

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    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 / energy-

    dispersive 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 electronmicroscopy 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.

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    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), dustsample 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

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    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 thismore 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

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    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).

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    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.

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    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.

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    Figure5: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.

    ***end of text***