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135Cs/137Cs Isotopic Ratio as a New Tracer of Radiocesium Released from the Fukushima Nuclear Accident

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† Research Center for Radiation Protection, National Institute of Radiological Sciences, 491 Anagawa, Inage, Chiba 263-8555, Japan
‡ State Key Laboratory of Nuclear Physics and Technology, School of Physics, Peking University, Beijing 100871, China
§ Project for Environmental Dynamics and Radiation Effects, Fukushima Project Headquarters, National Institute of Radiological Sciences, 491 Anagawa, Inage, Chiba 263-8555, Japan
∥ Department of Biology, Ohu University, 31-1 Koriyama, Fukushima 963-8611, Japan
*Telephone: 81-043-206-4634. Fax: 81-043-255-0721. E-mail: [email protected]
Cite this: Environ. Sci. Technol. 2014, 48, 10, 5433–5438
Publication Date (Web):April 29, 2014
https://doi.org/10.1021/es500403h
Copyright © 2014 American Chemical Society
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Abstract

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Since the Fukushima Daiichi nuclear power plant (FDNPP) accident in 2011, intensive studies of the distribution of released fission products, in particular 134Cs and 137Cs, in the environment have been conducted. However, the release sources, that is, the damaged reactors or the spent fuel pools, have not been identified, which resulted in great variation in the estimated amounts of 137Cs released. Here, we investigated heavily contaminated environmental samples (litter, lichen, and soil) collected from Fukushima forests for the long-lived 135Cs (half-life of 2 × 106 years), which is usually difficult to measure using decay-counting techniques. Using a newly developed triple-quadrupole inductively coupled plasma tandem mass spectrometry method, we analyzed the 135Cs/137Cs isotopic ratio of the FDNPP-released radiocesium in environmental samples. We demonstrated that radiocesium was mainly released from the Unit 2 reactor. Considering the fact that the widely used tracer for the released Fukushima accident-sourced radiocesium in the environment, the 134Cs/137Cs activity ratio, will become unavailable in the near future because of the short half-life of 134Cs (2.06 years), the 135Cs/137Cs isotopic ratio can be considered as a new tracer for source identification and long-term estimation of the mobility of released radiocesium in the environment.

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Effect of N2O gas flow rate on the signal intensity of 133Cs and 137Ba using Agilent 8800 triple-quadrupole ICP-MS/MS (Figure S1). This material is available free of charge via the Internet at http://pubs.acs.org.

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