A Method of Measurement of 239Pu, 240Pu, 241Pu in High U Content Marine Sediments by Sector Field ICP–MS and Its Application to Fukushima Sediment Samples
- Wenting Bu ,
- Jian Zheng ,
- Qiuju Guo ,
- Tatsuo Aono ,
- Hirofumi Tazoe ,
- Keiko Tagami ,
- Shigeo Uchida , and
- Masatoshi Yamada
Abstract

An accurate and precise analytical method is highly needed for the determination of Pu isotopes in marine sediments for the long-term marine environment monitoring that is being done since the Fukushima Dai-ichi Nuclear Power Plant accident. The elimination of uranium from the sediment samples needs to be carefully checked. We established an analytical method based on anion-exchange chromatography and SF-ICP–MS in this work. A uranium decontamination factor of 2 × 106 was achieved, and the U concentrations in the final sample solutions were typically below 4 pg mL–1, thus no extra correction of 238U interferences from the Pu spectra was needed. The method was suitable for the analysis of 241Pu in marine sediments using large sample amounts (>10 g). We validated the method by measuring marine sediment reference materials and our results agreed well with the certified and the literature values. Surface sediments and one sediment core sample collected after the nuclear accident were analyzed. The characterization of 241Pu/239Pu atom ratios in the surface sediments and the vertical distribution of Pu isotopes showed that there was no detectable Pu contamination from the nuclear accident in the marine sediments collected 30 km off the plant site.
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- Zhongtang Wang, Jian Zheng, Liguo Cao, Keiko Tagami, and Shigeo Uchida . Method for Ultratrace Level 241Am Determination in Large Soil Samples by Sector Field-Inductively Coupled Plasma Mass Spectrometry: With Emphasis on the Removal of Spectral Interferences and Matrix Effect. Analytical Chemistry 2016, 88 (14) , 7387-7394. https://doi.org/10.1021/acs.analchem.6b01934
- Zhongtang Wang, Guosheng Yang, Jian Zheng, Liguo Cao, Haijun Yu, Yanbei Zhu, Keiko Tagami, and Shigeo Uchida . Effect of Ashing Temperature on Accurate Determination of Plutonium in Soil Samples. Analytical Chemistry 2015, 87 (11) , 5511-5515. https://doi.org/10.1021/acs.analchem.5b01472
- Wenting Bu, Miho Fukuda, Jian Zheng, Tatsuo Aono, Takashi Ishimaru, Jota Kanda, Guosheng Yang, Keiko Tagami, Shigeo Uchida, Qiuju Guo, and Masatoshi Yamada . Release of Pu Isotopes from the Fukushima Daiichi Nuclear Power Plant Accident to the Marine Environment Was Negligible. Environmental Science & Technology 2014, 48 (16) , 9070-9078. https://doi.org/10.1021/es502480y
- Junwen Wu, Jian Zheng, Minhan Dai, Chih-An Huh, Weifang Chen, Keiko Tagami, and Shigeo Uchida . Isotopic Composition and Distribution of Plutonium in Northern South China Sea Sediments Revealed Continuous Release and Transport of Pu from the Marshall Islands. Environmental Science & Technology 2014, 48 (6) , 3136-3144. https://doi.org/10.1021/es405363q
- 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
- Miting Du, Tom D. Hylton, Sharon M. Robinson. Chemical processes for recovery and purification of high-purity uranium-234 from aged plutonium-238. Journal of Radioanalytical and Nuclear Chemistry 2021, 327 (1) , 417-424. https://doi.org/10.1007/s10967-020-07502-0
- Zhiyong Liu, Jun Hu, Masatoshi Yamada, Guosheng Yang. Uranium and plutonium isotopes and their environmental implications in surface sediments from the Yangtze River catchment and estuary. CATENA 2020, 193 , 104605. https://doi.org/10.1016/j.catena.2020.104605
- Junwen Wu, Jian Zheng. Reference materials for quality assurance of environmental plutonium analysis. Journal of Radioanalytical and Nuclear Chemistry 2020, 324 (1) , 169-188. https://doi.org/10.1007/s10967-020-07053-4
- Rui Zhang, Ruirui Wang, Zhiyong Liu, Fan Zhang, Tiegang Li, Minglei Guan, Qi Han. Distribution and transport of plutonium in the sediments of the Yangtze River estuary and the adjacent East China Sea. Applied Geochemistry 2020, 115 , 104532. https://doi.org/10.1016/j.apgeochem.2020.104532
- Yongjin Guan, Jingyu Mai, Jiawei Xu, Zhiyong Liu. Characteristic of Pu from urban wetland and lacustrine sediments in Suzhou Industrial Park, China. Journal of Environmental Radioactivity 2020, 213 , 106134. https://doi.org/10.1016/j.jenvrad.2019.106134
- Clemens Walther, Klaus Wendt. Radioisotope mass spectrometry. 2020,,, 861-898. https://doi.org/10.1016/B978-0-12-814397-1.00008-X
- . Handbook of Radioactivity Analysis. 2020,,https://doi.org/
- Zhongtang Wang, Zhaoya Huang, Yun Xie, Zhaoyi Tan. Method for determination of Pu isotopes in soil and sediment samples by inductively coupled plasma mass spectrometry after simple chemical separation using TK200 resin. Analytica Chimica Acta 2019, 1090 , 151-158. https://doi.org/10.1016/j.aca.2019.08.063
- Junwen Wu. Isotopic composition and source of plutonium in the Qinghai-Tibet Plateau frozen soils. Scientific Reports 2019, 9 (1) https://doi.org/10.1038/s41598-019-44391-0
- Junwen Wu, Minhan Dai, Yi Xu, Jian Zheng. Plutonium in the western North Pacific: Transport along the Kuroshio and implication for the impact of Fukushima Daiichi Nuclear Power Plant accident. Chemical Geology 2019, 511 , 256-264. https://doi.org/10.1016/j.chemgeo.2018.12.006
- 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
- 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
- Kexin Zhang, Guosheng Li, Shaoming Pan, Xiaoqing Qian, Zhiyong Liu, Yihong Xu, Yongpei Hao. Migration path and isotope tracing of 137Cs and 239 + 240Pu in estuary sediments: a case study of Liao River estuary in China. Journal of Soils and Sediments 2019, 19 (1) , 491-500. https://doi.org/10.1007/s11368-018-2092-2
- Youyi Ni, Zhongtang Wang, Jian Zheng, Keiko Tagami, Qiuju Guo, Shigeo Uchida, Hirofumi Tsukada. The transfer of fallout plutonium from paddy soil to rice: A field study in Japan. Journal of Environmental Radioactivity 2019, 196 , 22-28. https://doi.org/10.1016/j.jenvrad.2018.10.010
- Junwen Wu. Sources and scavenging of plutonium in the East China Sea. Marine Pollution Bulletin 2018, 135 , 808-818. https://doi.org/10.1016/j.marpolbul.2018.08.014
- 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
- Zhongtang Wang, Wei Wen, Wei Quan, Liang Du, Ping Wang, Jinxian Lin, Yun Xie, Zhaoyi Tan. Rapid determination of Pu isotopes for decommission concrete samples by inductively coupled plasma mass spectrometry. Journal of Radioanalytical and Nuclear Chemistry 2018, 316 (1) , 411-417. https://doi.org/10.1007/s10967-018-5756-x
- Jixin Qiao, Petra Lagerkvist, Ilia Rodushkin, Susanna Salminen-Paatero, Per Roos, Syverin Lierhagen, Karl Andreas Jensen, Emma Engstrom, Yann Lahaye, Lindis Skipperud. On the application of ICP-MS techniques for measuring uranium and plutonium: a Nordic inter-laboratory comparison exercise. Journal of Radioanalytical and Nuclear Chemistry 2018, 315 (3) , 565-580. https://doi.org/10.1007/s10967-018-5697-4
- Youyi Ni, Jian Zheng, Qiuju Guo, Hai Wang, Keiko Tagami, Shigeo Uchida. Comparisons of soil pretreatment methods for SF-ICP-MS determination of ultra-trace level plutonium in water soluble and exchangeable fractions. Journal of Radioanalytical and Nuclear Chemistry 2018, 315 (3) , 643-651. https://doi.org/10.1007/s10967-018-5700-0
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- Junwen Wu, Minhan Dai, Yi Xu, Jian Zheng. Sources and accumulation of plutonium in a large Western Pacific marginal sea: The South China Sea. Science of The Total Environment 2018, 610-611 , 200-211. https://doi.org/10.1016/j.scitotenv.2017.07.226
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- Wenting Bu, Qiuju Guo, Jian Zheng, Shigeo Uchida. Plutonium concentration and 240Pu/239Pu isotopic ratio in the surface soils from the Jiuquan region in northwestern China. Journal of Radioanalytical and Nuclear Chemistry 2017, 311 (2) , 999-1005. https://doi.org/10.1007/s10967-016-5002-3
- 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
- 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
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- 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
- Wenting Bu, Jian Zheng, Qiuju Guo, Tatsuo Aono, Shigeyoshi Otosaka, Keiko Tagami, Shigeo Uchida. Temporal distribution of plutonium isotopes in marine sediments off Fukushima after the Fukushima Dai-ichi Nuclear Power Plant accident. Journal of Radioanalytical and Nuclear Chemistry 2015, 303 (2) , 1151-1154. https://doi.org/10.1007/s10967-014-3437-y
- 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
- J. Zheng. Evaluation of a new sector-field ICP-MS with Jet Interface for ultra-trace determination of Pu isotopes: from femtogram to attogram levels. Journal of Nuclear and Radiochemical Sciences 2015, 15 (1) , 1_7-1_13. https://doi.org/10.14494/jnrs.15.1_7
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