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Novel Insights into Fukushima Nuclear Accident from Isotopic Evidence of Plutonium Spread along Coastal Rivers

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† Laboratoire des Sciences du Climat et de l’Environnement (LSCE/IPSL), Unité Mixte de Recherche 8212 (CEA/CNRS/UVSQ), 91198 Gif-sur-Yvette Cedex, France
‡ CEA, DAM, DIF, 91297 Arpajon, France
§ Center for Research in Isotopes and Environmental Dynamics, University of Tsukuba, Tsukuba 305-8572, Japan
∥ George Lemaître Centre for Earth and Climate Research, Earth & Life Institute, Université Catholique de Louvain, Louvain-la-Neuve, 1348, Belgium
*Phone: +33-1-69-82-35-20; e-mail: [email protected]
*Phone: +33-1-69-26-49-17; e-mail: [email protected]
Cite this: Environ. Sci. Technol. 2014, 48, 16, 9334–9340
Publication Date (Web):July 11, 2014
https://doi.org/10.1021/es501890n
Copyright © 2014 American Chemical Society
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Abstract

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The Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident led to important releases of radionuclides into the environment, and trace levels of plutonium (Pu) were detected in northeastern Japan. However, measurements of Pu isotopic atom and activity ratios are required to differentiate between the contributions of global nuclear test fallout and FDNPP emissions. In this study, we used a double-focusing sector field ICP–MS to measure Pu atom and activity ratios in recently deposited sediment along rivers draining the most contaminated part of the inland radioactive plume. Results showed that plutonium isotopes (i.e., 239Pu, 240Pu, 241Pu, and 242Pu) were detected in all samples, although in extremely low concentrations. The 241Pu/239Pu atom ratios measured in sediment deposits (0.0017–0.0884) were significantly higher than the corresponding values attributed to the global fallout (0.00113 ± 0.00008 on average for the Northern Hemisphere between 31°–71° N: Kelley, J. M.; Bond, L. A.; Beasley, T. M. Global distribution of Pu isotopes and 237Np. Sci. Total. Env. 1999, 237/238, 483–500). The results indicated the presence of Pu from FDNPP, in slight excess compared to the Pu background from global fallout that represented up to ca. 60% of Pu in the analyzed samples. These results demonstrate that this radionuclide has been transported relatively long distances (∼45 km) from FDNPP and been deposited in rivers representing a potential source of Pu to the ocean. In future, the high 241Pu/239Pu atom ratio of the Fukushima accident sourced-Pu should be measured to quantify the supply of continental-originating material from Fukushima Prefecture to the Pacific Ocean.

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Figure displaying the location of the analyzed samples on a map of 110mAg:137Cs activity ratio in soils of Fukushima Prefecture, and tables detailing the Pu isotopic composition used for calculation of the fraction of Pu from FDNPP in the analyzed soil samples (Table S1) and the results of Pu isotopic measurements carried out on Japanese soil samples or atmospheric deposition samples in Japan (Table S2). This material is available free of charge via the Internet at http://pubs.acs.org.

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Cited By

This article is cited by 28 publications.

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  15. C.C.S. Wendel, O.C. Lind, L.K. Fifield, S.G. Tims, B. Salbu, D.H. Oughton. No Fukushima Dai-ichi derived plutonium signal in marine sediments collected 1.5–57 km from the reactors. Applied Radiation and Isotopes 2017, 129 , 180-184. https://doi.org/10.1016/j.apradiso.2017.08.015
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  17. Liguo Cao, Jian Zheng, Hirofumi Tsukada, Shaoming Pan, Zhongtang Wang, Keiko Tagami, Shigeo Uchida. Simultaneous determination of radiocesium (135Cs, 137Cs) and plutonium (239Pu, 240Pu) isotopes in river suspended particles by ICP-MS/MS and SF-ICP-MS. Talanta 2016, 159 , 55-63. https://doi.org/10.1016/j.talanta.2016.06.008
  18. Liguo Cao, Wenting Bu, Jian Zheng, Shaoming Pan, Zhongtang Wang, Shigeo Uchida. Plutonium determination in seawater by inductively coupled plasma mass spectrometry: A review. Talanta 2016, 151 , 30-41. https://doi.org/10.1016/j.talanta.2016.01.010
  19. Yuji Shibahara, Takumi Kubota, Toshiyuki Fujii, Satoshi Fukutani, Koichi Takamiya, Mitsuyuki Konno, Satoshi Mizuno, Hajimu Yamana. Determination of isotopic ratios of plutonium and uranium in soil samples by thermal ionization mass spectrometry. Journal of Radioanalytical and Nuclear Chemistry 2016, 307 (3) , 2281-2287. https://doi.org/10.1007/s10967-015-4551-1
  20. Hugo Lepage, J. Patrick Laceby, Philippe Bonté, Jean-Louis Joron, Yuichi Onda, Irène Lefèvre, Sophie Ayrault, Olivier Evrard. Investigating the source of radiocesium contaminated sediment in two Fukushima coastal catchments with sediment tracing techniques. Anthropocene 2016, 13 , 57-68. https://doi.org/10.1016/j.ancene.2016.01.004
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