Release of Pu Isotopes from the Fukushima Daiichi Nuclear Power Plant Accident to the Marine Environment Was Negligible
- Wenting Bu ,
- Miho Fukuda ,
- Jian Zheng ,
- Tatsuo Aono ,
- Takashi Ishimaru ,
- Jota Kanda ,
- Guosheng Yang ,
- Keiko Tagami ,
- Shigeo Uchida ,
- Qiuju Guo , and
- Masatoshi Yamada
Abstract

Atmospheric deposition of Pu isotopes from the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident has been observed in the terrestrial environment around the FDNPP site; however, their deposition in the marine environment has not been studied. The possible contamination of Pu in the marine environment has attracted great scientific and public concern. To fully understand this possible contamination of Pu isotopes from the FDNPP accident to the marine environment, we collected marine sediment core samples within the 30 km zone around the FDNPP site in the western North Pacific about two years after the accident. Pu isotopes (239Pu, 240Pu, and 241Pu) and radiocesium isotopes (134Cs and 137Cs) in the samples were determined. The high activities of radiocesium and the 134Cs/137Cs activity ratios with values around 1 (decay corrected to 15 March 2011) suggested that these samples were contaminated by the FDNPP accident-released radionuclides. However, the activities of 239+240Pu and 241Pu were low compared with the background level before the FDNPP accident. The Pu atom ratios (240Pu/239Pu and 241Pu/239Pu) suggested that global fallout and the pacific proving ground (PPG) close-in fallout are the main sources for Pu contamination in the marine sediments. As Pu isotopes are particle-reactive and they can be easily incorporated with the marine sediments, we concluded that the release of Pu isotopes from the FDNPP accident to the marine environment was negligible.
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- Hugo Jaegler, Alkiviadis Gourgiotis, Peter Steier, Robin Golser, Olivier Diez, Charlotte Cazala. Pushing Limits of ICP–MS/MS for the Determination of Ultralow 236U/238U Isotope Ratios. Analytical Chemistry 2020, 92 (11) , 7869-7876. https://doi.org/10.1021/acs.analchem.0c01121
- Núria Casacuberta, Marcus Christl, Ken O. Buesseler, YikSze Lau, Christof Vockenhuber, Maxi Castrillejo, Hans-Arno Synal, and Pere Masqué . Potential Releases of 129I, 236U, and Pu Isotopes from the Fukushima Dai-ichi Nuclear Power Plants to the Ocean from 2013 to 2015. Environmental Science & Technology 2017, 51 (17) , 9826-9835. https://doi.org/10.1021/acs.est.7b03057
- Karin Hain, Thomas Faestermann, Leticia Fimiani, Robin Golser, José Manuel Gómez-Guzmán, Gunther Korschinek, Florian Kortmann, Christoph Lierse von Gostomski, Peter Ludwig, Peter Steier, Hirofumi Tazoe, and Masatoshi Yamada . Plutonium Isotopes (239–241Pu) Dissolved in Pacific Ocean Waters Detected by Accelerator Mass Spectrometry: No Effects of the Fukushima Accident Observed. Environmental Science & Technology 2017, 51 (4) , 2031-2037. https://doi.org/10.1021/acs.est.6b05605
- Brett L. Rosenberg, Katsumi Shozugawa, and Georg Steinhauser . Detection of Fuel Release in a Nuclear Accident: A Method for Preconcentration and Isolation of Reactor-Borne 239Np Using Ion-Specific Extraction Chromatography. Analytical Chemistry 2015, 87 (17) , 8651-8656. https://doi.org/10.1021/acs.analchem.5b02265
- Liguo Cao, Jian Zheng, Zhengchao Zhou, Wenting Bu, Zhongtang Wang, Wang Zheng, Masatoshi Yamada. Distribution and behavior of plutonium isotopes in Western Pacific marginal seas. CATENA 2021, 198 , 105023. https://doi.org/10.1016/j.catena.2020.105023
- Masatoshi Yamada, Shinji Oikawa, Yuhei Shirotani, Masashi Kusakabe, Koji Shindo. Transuranic nuclides Pu, Am and Cm isotopes, and 90Sr in seafloor sediments off the Fukushima Daiichi Nuclear Power Plant during the period from 2012 to 2019. Journal of Environmental Radioactivity 2021, 227 , 106459. https://doi.org/10.1016/j.jenvrad.2020.106459
- Yukun Fan, Xiaolin Hou, Miho Fukuda, Jian Zheng, Tatsuo Aono, Ning Chen, Luyuan Zhang, Weijian Zhou. 129I in a sediment core offshore Fukushima: Distribution, source and its implication. Chemosphere 2020, 252 , 126524. https://doi.org/10.1016/j.chemosphere.2020.126524
- Youyi Ni, Qiuju Guo, Zhaoya Huang, Jian Zheng, Sixuan Li, Wenna Huang, Wenting Bu. First study of 237Np in Chinese soils: Source, distribution and mobility in comparison with plutonium isotopes. Chemosphere 2020, 253 , 126683. https://doi.org/10.1016/j.chemosphere.2020.126683
- Wang Jinlong, Du Jinzhou, Zheng Jian. Plutonium Isotopes Research in the Marine Environment: A synthesis. Journal of Nuclear and Radiochemical Sciences 2020, 20 (0) , 1-11. https://doi.org/10.14494/jnrs.20.1
- Yuki Morishita, Tatsuo Torii, Hiroshi Usami, Hiroyuki Kikuchi, Wataru Utsugi, Shiro Takahira. Detection of alpha particle emitters originating from nuclear fuel inside reactor building of Fukushima Daiichi Nuclear Power Plant. Scientific Reports 2019, 9 (1) https://doi.org/10.1038/s41598-018-36962-4
- Daisuke Tsumune, Jota Kanda. Environmental Dynamics and Future Projection of Radioactive Materials in the Ocean. RADIOISOTOPES 2019, 68 (11) , 793-803. https://doi.org/10.3769/radioisotopes.68.793
- Wu Men, Jian Zheng, Hai Wang, Youyi Ni, Yuichiro Kumamoto, Masatoshi Yamada, Shigeo Uchida. Pu isotopes in the seawater off Fukushima Daiichi Nuclear Power Plant site within two months after the severe nuclear accident. Environmental Pollution 2019, 246 , 303-310. https://doi.org/10.1016/j.envpol.2018.12.007
- Wenting Bu, Lei Tang, Xuemei Liu, Zhongtang Wang, Miho Fukuda, Jian Zheng, Tatsuo Aono, Sheng Hu, Xiaolin Wang. Ultra-trace determination of the 135 Cs/ 137 Cs isotopic ratio by thermal ionization mass spectrometry with application to Fukushima marine sediment samples. Journal of Analytical Atomic Spectrometry 2019, 34 (2) , 301-309. https://doi.org/10.1039/C8JA00380G
- Youyi Ni, Jian Zheng, Qiuju Guo, Hai Wang. The Key Role of Isotopic Analysis in Tracing the Fukushima Nuclear Accident-Released Pu and Radiocesium Isotopes in the Environment. 2019,,, 163-173. https://doi.org/10.1007/978-981-13-8327-4_14
- , , . Nuclear Emergencies. 2019,,https://doi.org/10.1007/978-981-13-8327-4
- Fei Chen, Jun Hu, Yoshio Takahashi, Masatoshi Yamada, M. Safiur Rahman, Guosheng Yang. Application of synchrotron radiation and other techniques in analysis of radioactive microparticles emitted from the Fukushima Daiichi Nuclear Power Plant accident-A review. Journal of Environmental Radioactivity 2019, 196 , 29-39. https://doi.org/10.1016/j.jenvrad.2018.10.013
- Yihong Xu, Shaoming Pan, Jianhua Gao, Xiaolin Hou, Yongfu Ma, Yongpei Hao. Sedimentary record of plutonium in the North Yellow Sea and the response to catchment environmental changes of inflow rivers. Chemosphere 2018, 207 , 130-138. https://doi.org/10.1016/j.chemosphere.2018.05.082
- Hugo Jaegler, Fabien Pointurier, Yuichi Onda, Amélie Hubert, J. Patrick Laceby, Maëva Cirella, Olivier Evrard. Plutonium isotopic signatures in soils and their variation (2011-2014) in sediment transiting a coastal river in the Fukushima Prefecture, Japan. Environmental Pollution 2018, 240 , 167-176. https://doi.org/10.1016/j.envpol.2018.04.094
- P. Thakur, A. L. Ward. 241Pu in the environment: insight into the understudied isotope of plutonium. Journal of Radioanalytical and Nuclear Chemistry 2018, 317 (2) , 757-778. https://doi.org/10.1007/s10967-018-5946-6
- Wijittra Wongjaikham, Doonyapong Wongsawaeng, Peter Hosemann, Chaiyaruang Kanokworakan, Vareeporn Ratnitsai. Enhancement of uranium recovery from seawater using amidoximated polymer gel synthesized from radiation-polymerization and crosslinking of acrylonitrile and methacrylic acid monomers. Journal of Environmental Chemical Engineering 2018, 6 (2) , 2768-2777. https://doi.org/10.1016/j.jece.2018.04.016
- Christiane Dufresne, Céline Duffa, Vincent Rey, Romaric Verney. Hydro-sedimentary model as a post-accidental management tool: Application to radionuclide marine dispersion in the Bay of Toulon (France). Ocean & Coastal Management 2018, 153 , 176-192. https://doi.org/10.1016/j.ocecoaman.2017.12.026
- Leslie Mendoza Temple, Pooja Saigal. Hypothyroidism. 2018,,, 347-360.e3. https://doi.org/10.1016/B978-0-323-35868-2.00034-7
- . Integrative Medicine. 2018,,https://doi.org/
- Wenting Bu, Youyi Ni, Georg Steinhauser, Wang Zheng, Jian Zheng, Naoki Furuta. The role of mass spectrometry in radioactive contamination assessment after the Fukushima nuclear accident. Journal of Analytical Atomic Spectrometry 2018, 33 (4) , 519-546. https://doi.org/10.1039/C7JA00401J
- Guosheng Yang, Yoshihisa Kato, Hirofumi Tazoe, Masatoshi Yamada. Applying an improved method to measure 134Cs, 135Cs, and 137Cs activities and their atom ratios in marine sediments collected close to the Fukushima Daiichi Nuclear Power Plant. GEOCHEMICAL JOURNAL 2018, 52 (2) , 219-226. https://doi.org/10.2343/geochemj.2.0484
- Guosheng Yang, Hirofumi Tazoe, Masatoshi Yamada. Can 129I track 135Cs, 236U, 239Pu, and 240Pu apart from 131I in soil samples from Fukushima Prefecture, Japan?. Scientific Reports 2017, 7 (1) https://doi.org/10.1038/s41598-017-15714-w
- 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
- Liguo Cao, Nobuyoshi Ishii, Jian Zheng, Maiko Kagami, Shaoming Pan, Keiko Tagami, Shigeo Uchida. Vertical distributions of Pu and radiocesium isotopes in sediments from Lake Inba after the Fukushima Daiichi Nuclear Power Plant accident: Source identification and accumulation. Applied Geochemistry 2017, 78 , 287-294. https://doi.org/10.1016/j.apgeochem.2017.01.012
- Shizuho Miki, Ken Fujimoto, Yuya Shigenobu, Daisuke Ambe, Hideki Kaeriyama, Kaori Takagi, Tsuneo Ono, Tomowo Watanabe, Hiroya Sugisaki, Takami Morita. Concentrations of 90 Sr and 137 Cs/ 90 Sr activity ratios in marine fishes after the Fukushima Dai-ichi Nuclear Power Plant accident. Fisheries Oceanography 2017, 26 (2) , 221-233. https://doi.org/10.1111/fog.12182
- Brit Salbu, Ole Christian Lind. Radioactive particles released to the environment from the Fukushima reactors-Confirmation is still needed. Integrated Environmental Assessment and Management 2016, 12 (4) , 687-689. https://doi.org/10.1002/ieam.1834
- Mei-Ling Tang, Ben-Jei Tsuang, Pei-Hsuan Kuo. Dose estimation for nuclear power plant 4 accident in Taiwan at Fukushima nuclear meltdown emission level. Journal of Environmental Radioactivity 2016, 155-156 , 71-83. https://doi.org/10.1016/j.jenvrad.2016.01.022
- 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
- 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
- WuHui Lin, LiQi Chen, Wen Yu, Hao Ma, Zhi Zeng, Shi Zeng. Radioactive source terms for the Fukushima nuclear accident. Science China Earth Sciences 2016, 59 (1) , 214-222. https://doi.org/10.1007/s11430-015-5112-8
- Shinji Oikawa, Teruhisa Watabe, Hyoe Takata. Distributions of Pu isotopes in seawater and bottom sediments in the coast of the Japanese archipelago before and soon after the Fukushima Dai-ichi Nuclear Power Station accident. Journal of Environmental Radioactivity 2015, 142 , 113-123. https://doi.org/10.1016/j.jenvrad.2015.01.003
- W. Lin, L. Chen, W. Yu, H. Ma, Z. Zeng, J. Lin, S. Zeng. Radioactivity impacts of the Fukushima Nuclear Accident on the atmosphere. Atmospheric Environment 2015, 102 , 311-322. https://doi.org/10.1016/j.atmosenv.2014.11.047
- W.T. Bu, J. Zheng, T. Aono, J.W. Wu, K. Tagami, S. Uchida, Q.J. Guo, M. Yamada. Pu Distribution in Seawater in the Near Coastal Area off Fukushima after the Fukushima Daiichi Nuclear Power Plant Accident. Journal of Nuclear and Radiochemical Sciences 2015, 15 (1) , 1_1-1_6. https://doi.org/10.14494/jnrs.15.1_1



