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Speciation of Radioactive Soil Particles in the Fukushima Contaminated Area by IP Autoradiography and Microanalyses

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† Department of Earth and Planetary Science, Graduate School of Science, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo, 113-0033, Japan
‡ Japan International Research Center for Agricultural Sciences, 1-1 Ohwashi, Tsukuba, Ibaraki 305-8686, Japan
§ Quantum Beam Unit, National Institute for Materials Science, 1-2-1 Sengen, Tsukuba, Ibaraki 305-0047, Japan
∥ Environmental Remediation Materials Unit, National Institute for Materials Science, 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan
⊥ Quantum Beam Science Center and Fukushima Environmental Safety Center, Japan Atomic Enegy Agency, 1-1-1 Kouto, Sayo-cho, Sayo-gun, Hyogo 679-5148, Japan
*Phone: +81-3-5841-4019; fax: +81-3-5841-4019; e-mail:[email protected]
Cite this: Environ. Sci. Technol. 2014, 48, 22, 13053–13059
Publication Date (Web):October 24, 2014
https://doi.org/10.1021/es502849e
Copyright © 2014 American Chemical Society
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Abstract

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Radioactive soil particles several tens of micrometers in size were collected from litter soil in the radiation contaminated area by the Fukushima nuclear plant accident and characterized using electron and X-ray microanalyses. The radioactive particles were discriminated by autoradiography using imaging plates (IP) on which microgrids were formed by laser ablation in order to find the particles under microscopy. Fifty radioactive particles were identified and classified into three types from their morphology and chemical composition, namely: (1) aggregates of clay minerals, (2) organic matter containing clay mineral particulates, and (3) weathered biotite originating from local granite. With respect to the second type, dissolution of the organic matter did not reduce the radiation, suggesting that the radionuclides were also fixed by the clay minerals. The weathered biotite grains have a plate-like shape with well-developed cleavages inside the grains, and kaolin group minerals and goethite filling the cleavage spaces. The reduction of the radiation intensity was measured before and after the trimming of the plate edges using a focused ion beam (FIB), to examine whether radioactive cesium primarily sorbed at frayed edges. The radiation was attenuated in proportion to the volume decrease by the edge trimming, implying that radioactive cesium was sorbed uniformly in the porous weathered biotite.

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Figure S1. γ-ray spectrums from the litter soil particles, collected from the ground of forest in the Fukushima contaminated area. Figure S2. (a) Eleven soil particles with possibility to be radioactive, picked up and transferred onto conductive double-stick tape. (b) Read-out image of an IP which covered the tape in (a) for a week. Figure S3. Examples of electron diffraction patterns obtained from the third type, e.g. radioactive plate-like particles, to confirm the mineral phases. Figure S4. SEM images (top), EDS spectra (center) and γ-ray spectra (bottom) from (a) the first type (aggregates of clay minerals) and (b) the second type (organic matter dominant) radioactive particles described in the text. This material is available free of charge via the Internet at http://pubs.acs.org.

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