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Development of mass spectrometric method for simultaneous determination of hard-to-measure Pu isotopes in environmental and reactor decommissioning waste samples

Research Project

Project/Area Number 17K00537
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeMulti-year Fund
Section一般
Research Field Environmental dynamic analysis
Research InstitutionNational Institutes for Quantum and Radiological Science and Technology

Principal Investigator

Zheng Jian  国立研究開発法人量子科学技術研究開発機構, 高度被ばく医療センター 福島再生支援研究部, 上席研究員(定常) (30370878)

Project Period (FY) 2017-04-01 – 2020-03-31
Project Status Completed (Fiscal Year 2019)
Budget Amount *help
¥4,420,000 (Direct Cost: ¥3,400,000、Indirect Cost: ¥1,020,000)
Fiscal Year 2019: ¥1,170,000 (Direct Cost: ¥900,000、Indirect Cost: ¥270,000)
Fiscal Year 2018: ¥1,300,000 (Direct Cost: ¥1,000,000、Indirect Cost: ¥300,000)
Fiscal Year 2017: ¥1,950,000 (Direct Cost: ¥1,500,000、Indirect Cost: ¥450,000)
KeywordsPu同位体 / トリプル四重極ICP-MS/MS / 環境動態解析 / 廃炉関連廃棄物 / 環境試料 / 新規低温溶融法 / 先端質量分析法 / Plutonium isotopes / ICP-MS/MS / Environmental samples / Nuclear Decommissioning / Low-temperature fusion / ICP-MS / Nuclear decommissioning / 環境計測
Outline of Final Research Achievements

In this study, we developed an advanced mass spectrometry method for simultaneous analysis of important Pu isotopes (238,239,240,241Pu) using triple quadrupole ICP-MS/MS by employing the ion-molecule reaction separate U-238 and Pu-238, which was previously difficult to be measured. By introducing a desolvation sample introduction system, we succeeded in increasing 10 times the sensitivity of Pu isotopes and suppressing the production of uranium hydride, we achieved the detection limit of fg level in on-mass mode. We have established a rapid analytical method for small volume seawater and developed a new low-temperature fusion method for environmental and nuclear decommissioning samples. By combining these new sample preparation techniques with the developed ICP-MS/MS detection, a rapid Pu isotope mass spectrometry method for environmental samples and decommissioning related waste samples was established.

Academic Significance and Societal Importance of the Research Achievements

東電福島第一原発事故由来Pu同位体の環境動態解析、環境除染・廃炉作業に伴い発生する廃棄物の汚染状況の把握及び被ばく線量の評価には、重要同位体(Pu-238,Pu-239,Pu-240,Pu-241)の測定が必要である。本研究で開発した環境と廃炉関連試料中Pu迅速質量分析法は環境に優しい方法であり、環境科学研究と原子力緊急時の対応まで幅広い応用を期待できる。

Report

(4 results)
  • 2019 Annual Research Report   Final Research Report ( PDF )
  • 2018 Research-status Report
  • 2017 Research-status Report
  • Research Products

    (45 results)

All 2020 2019 2018 2017 Other

All Int'l Joint Research (5 results) Journal Article (18 results) (of which Int'l Joint Research: 16 results,  Peer Reviewed: 18 results,  Open Access: 2 results) Presentation (21 results) (of which Int'l Joint Research: 12 results,  Invited: 11 results) Book (1 results)

  • [Int'l Joint Research] Peking University/Third Institute of Oceanography/Shantou University(中国)

    • Related Report
      2019 Annual Research Report
  • [Int'l Joint Research] 北京大学物理学部/第三海洋研究所/南華大学原子核科学技術学部(中国)

    • Related Report
      2018 Research-status Report
  • [Int'l Joint Research] Arizona State University/Savannah River National Laboratory/Metropolitan State University of Denver(米国)

    • Related Report
      2017 Research-status Report
  • [Int'l Joint Research] Leibniz University Hannover(ドイツ)

    • Related Report
      2017 Research-status Report
  • [Int'l Joint Research] 北京大学物理学部/Third Institute of Oceanography/University of South China(中国)

    • Related Report
      2017 Research-status Report
  • [Journal Article] First study of 237Np in Chinese soils: Source, distribution and mobility in comparison with plutonium isotopes2020

    • Author(s)
      Ni Youyi、Guo Qiuju、Huang Zhaoya、Zheng Jian、Li Sixuan、Huang Wenna、Bu Wenting
    • Journal Title

      Chemosphere

      Volume: 253 Pages: 126683-126683

    • DOI

      10.1016/j.chemosphere.2020.126683

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Reference materials for quality assurance of environmental plutonium analysis2020

    • Author(s)
      Junwen Wu, Jian Zheng
    • Journal Title

      Journal of Radioanalytical and Nuclear Chemistry

      Volume: 324 Issue: 1 Pages: 169-188

    • DOI

      10.1007/s10967-020-07053-4

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Plutonium isotopes research in the marine environment: A synthesis2020

    • Author(s)
      Jinlong Wang, Jinzhou Du, Jian Zheng
    • Journal Title

      Journal of Nuclear and Radiochemical Science

      Volume: 20 Pages: 1-11

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Simultaneous determination of ultra-trace level 237Np and Pu isotopes in soil and sediment samples by SF-ICP-MS with a single column chromatographic separation2019

    • Author(s)
      Zhaoya Huang, Youyi Ni, Hai Wang, Jian Zheng, Shinnosuke yamazaki, Aya Sakaguchi, Xinggui Long, Shigeo Uchida
    • Journal Title

      Microchemical Journal

      Volume: 148 Pages: 597-604

    • DOI

      10.1016/j.microc.2019.05.044

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Pu isotopes in seawater off Fukushima Daiichi Nuclear Power Plant site within tw months after the severe nuclear accident2019

    • Author(s)
      W. Men, J. Zheng*, H. Wang, Y. Y. Ni, Y. Kumamoto, M. Yamada, S. Uchida
    • Journal Title

      Environmental Pollution

      Volume: 246 Pages: 303-310

    • DOI

      10.1016/j.envpol.2018.12.007

    • Related Report
      2019 Annual Research Report 2018 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Environmental impact and food safety in Japan after the Fukushima Daiichi Nuclear Power Plant accident2019

    • Author(s)
      Guosheng Yang, Jun Hu, Jian Zheng
    • Journal Title

      Int. J. Radiat. Med. Nucl. Med.

      Volume: 43 Pages: 99-105

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] First determination of Pu isotopes (239Pu, 240Pu and 241Pu) in radioactive particles derived from Fukushima Daiichi Nuclear Power Plant accident2019

    • Author(s)
      Igarashi Junya、Zheng Jian、Zhang Zijian、Ninomiya Kazuhiko、Satou Yukihiko、Fukuda Miho、Ni Youyi、Aono Tatsuo、Shinohara Atsushi
    • Journal Title

      Scientific Reports

      Volume: 9 Issue: 1 Pages: 11807-11807

    • DOI

      10.1038/s41598-019-48210-4

    • NAID

      120006763792

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Low-temperature fusion using NH4HSO4 and NH4HF2 for rapid determination of Pu in soil and sediment samples2019

    • Author(s)
      Wang Hai、Ni Youyi、Zheng Jian、Huang Zhaoya、Xiao Detao、Aono Tatsuo
    • Journal Title

      Analytica Chimica Acta

      Volume: 1050 Pages: 71-79

    • DOI

      10.1016/j.aca.2018.10.065

    • Related Report
      2018 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Plutonium in the western North Pacific: Transport along the Kuroshio and implication for the impact of Fukushima Daiichi Nuclear Power Plant accident2019

    • Author(s)
      Wu Junwen、Dai Minhan、Xu Yi、Zheng Jian
    • Journal Title

      Chemical Geology

      Volume: 511 Pages: 256-264

    • DOI

      10.1016/j.chemgeo.2018.12.006

    • Related Report
      2018 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Ultra-trace determination of the 135Cs/137Cs isotopic ratio by thermal ionization mass spectrometry with application to Fukushima marine sediment samples2019

    • Author(s)
      Bu Wenting、Tang Lei、Liu Xuemei、Wang Zhongtang、Fukuda Miho、Zheng Jian、Aono Tatsuo、Hu Sheng、Wang Xiaolin
    • Journal Title

      Journal of Analytical Atomic Spectrometry

      Volume: 34 Issue: 2 Pages: 301-309

    • DOI

      10.1039/c8ja00380g

    • Related Report
      2018 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] The transfer of fallout plutonium from paddy soil to rice: A field study in Japan2019

    • Author(s)
      Ni Youyi、Wang Zhongtang、Zheng Jian、Tagami Keiko、Guo Qiuju、Uchida Shigeo、Tsukada Hirofumi
    • Journal Title

      Journal of Environmental Radioactivity

      Volume: 196 Pages: 22-28

    • DOI

      10.1016/j.jenvrad.2018.10.010

    • Related Report
      2018 Research-status Report
    • Peer Reviewed
  • [Journal Article] Distinctive distributions and migrations of 239+240Pu and 241Am in Chinese forest, grassland and desert soils2018

    • Author(s)
      Ni Youyi、Wang Zhongtang、Guo Qiuju、Zheng Jian、Li Sixuan、Lin Jinxian、Tan Zhaoyi、Huang Wenna
    • Journal Title

      Chemosphere

      Volume: 212 Pages: 1002-1009

    • DOI

      10.1016/j.chemosphere.2018.09.021

    • Related Report
      2018 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Rapid determination of ultra-trace plutonium isotopes ( 239 Pu, 240 Pu and 241 Pu) in small-volume human urine bioassay using sector-field inductively coupled plasma mass spectrometry2018

    • Author(s)
      Ni Youyi、Zheng Jian、Guo Qiuju、Men Wu、Tagami Keiko、Uchida Shigeo
    • Journal Title

      Analytica Chimica Acta

      Volume: 1000 Pages: 85-92

    • DOI

      10.1016/j.aca.2017.10.012

    • Related Report
      2017 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Establishing rapid analysis of Pu isotopes in seawater to study the impact of Fukushima nuclear accident in the Northwest Pacific2018

    • Author(s)
      Men Wu、Zheng Jian、Wang Hai、Ni Youyi、Aono Tatsuo、Maxwell Sherrod L.、Tagami Keiko、Uchida Shigeo、Yamada Masatoshi
    • Journal Title

      Scientific Reports

      Volume: 8 Issue: 1 Pages: 1-11

    • DOI

      10.1038/s41598-018-20151-4

    • Related Report
      2017 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] The role of mass spectrometry in radioactive contamination assessment after the Fukushima nuclear accident2018

    • Author(s)
      Bu Wenting、Ni Youyi、Steinhauser Georg、Zheng Wang、Zheng Jian、Furuta Naoki
    • Journal Title

      Journal of Analytical Atomic Spectrometry

      Volume: 33 Issue: 4 Pages: 519-546

    • DOI

      10.1039/c7ja00401j

    • Related Report
      2017 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] A rapid method for accurate determination of 241Am by sector field inductively coupled plasma mass spectrometry and its application to Sellafield site soil samples2017

    • Author(s)
      Wang Z. T.、Zheng J.、Imanaka T.、Uchida S.
    • Journal Title

      Journal of Analytical Atomic Spectrometry

      Volume: 32 Issue: 10 Pages: 2034-2040

    • DOI

      10.1039/c7ja00201g

    • Related Report
      2017 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Development and application of mass spectrometric techniques for ultra-trace determination of 236 U in environmental samples-A review2017

    • Author(s)
      Bu Wenting、Zheng Jian、Ketterer Michael E.、Hu Sheng、Uchida Shigeo、Wang Xiaolin
    • Journal Title

      Analytica Chimica Acta

      Volume: 995 Pages: 1-20

    • DOI

      10.1016/j.aca.2017.09.029

    • Related Report
      2017 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Determination of Pu isotopes in sediment and soil samples by SF-ICP-MS: an improved anion-exchange procedure for Pu separation2017

    • Author(s)
      Bu Wenting、Zheng Jian、Guo Qiuju、Xiao Detao、Aono Tatsuo
    • Journal Title

      Journal of Radioanalytical and Nuclear Chemistry

      Volume: 314 Issue: 3 Pages: 2417-2423

    • DOI

      10.1007/s10967-017-5618-y

    • Related Report
      2017 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Presentation] 福島原発事故により放出されたタイプの異なる不溶性粒子のSr, Pu分析2020

    • Author(s)
      五十嵐淳哉,鄭 建,張子見, 二宮和彦, 佐藤志彦, 福田美保,倪 有意,青野辰雄,末木啓介,篠原厚
    • Organizer
      第21回「環境放射能研究会」
    • Related Report
      2019 Annual Research Report
  • [Presentation] Reference materials for quality assurance of plutonium isotope ratio analysis in environmental samples2020

    • Author(s)
      Junwen Wu, Jian Zheng
    • Organizer
      第21回「環境放射能研究会」
    • Related Report
      2019 Annual Research Report
  • [Presentation] Tracing the Fukushima nuclear accident released radiocesium and Pu isotopes in the environment: the role of isotope ratio analysis2019

    • Author(s)
      Jian Zheng
    • Organizer
      The 10th National Conference on Environmental Chemistry, China
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Recent progress on mass spectrometric analysis of ultra-trace radioactive isotopes2019

    • Author(s)
      Jian Zheng
    • Organizer
      The workshop on radioactive isotopes analysis, Taiyuan, China
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Rapid method for ultra-trace urinary plutonium bioassay with inductively coupled plasma mass spectrometry2019

    • Author(s)
      Jian Zheng, Guosheng Yang, Eunjoo Kim, Osamu Kurihara
    • Organizer
      The 5th ARADOS annual meeting, Beijing, China
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Development of low-temperature fusion using ammonium hydrogen fluoride for rapid determination of actinides in environmental and nuclear decommissioning samples2019

    • Author(s)
      Jian Zheng, Hai Wang, Zhaoya Huang, Youyi Ni, Tatsuo Aono
    • Organizer
      日本分析化学会第68年会
    • Related Report
      2019 Annual Research Report
  • [Presentation] 福島原発事故により放出された不溶性粒子に含まれるプルトニウムの定量2019

    • Author(s)
      五十嵐淳哉,鄭 建, 張 子見, 二宮和彦, 佐藤志彦, 福田美保, 倪 有意, 青野辰雄, 篠原厚
    • Organizer
      日本放射化学会第63回討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Identification of Plutonium isotopes in radioactive particles released from the Fukushima Daiichi Nuclear Power Plant2019

    • Author(s)
      Junya Igarashi, Jian Zheng, Zhijian Zhang, Kazuhiko Ninomiya, Yukihiko Satou, Miho Fukuda, Youyi Ni, Tatsuo Aono
    • Organizer
      5th International conference on Environmental Radioactivity Variations of Environmental radionuclides
    • Related Report
      2019 Annual Research Report
  • [Presentation] 福島第一原発事故後の陸域環境中のネプツニウムとプルトニウムについて2019

    • Author(s)
      福田 美保, 鄭 建, 山崎 慎之介, 青野 辰雄
    • Organizer
      第20回「環境放射能研究会」, 高エネルギー加速器研究機構放射線科学センター
    • Related Report
      2018 Research-status Report
  • [Presentation] Low-temperature fusion using NH4HF2 for rapid determination of Pu isotopes by ICP-MS/MS: application for marine sediments collected in Japanese coast2019

    • Author(s)
      Jian Zheng, Hai Wang, Zhaoya Huang, Youyi Ni, Tatsuo Aono
    • Organizer
      第20回「環境放射能研究会」, 高エネルギー加速器研究機構放射線科学センター
    • Related Report
      2018 Research-status Report
  • [Presentation] Ultra-trace measurement of radioactive isotopes using mass spectrometry2018

    • Author(s)
      鄭 建
    • Organizer
      Japan-Korea Technology Information Exchange Seminar 2018, Japan Analytical Instruments Manufacturers's Association (JAIMA), Japan (招待講演)
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Plutonium isotopes in seawater off Fukushima within two months after the accident2018

    • Author(s)
      Jian Zheng, Wu Men, Hai Wang, Yuichiro Kumamoto, Masatoshi Yamada, Shigeo Uchida
    • Organizer
      Goldschmidt 2018, Geochemical Society and the European Association of Geochemistry(招待講演)(国際学会)
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Rapid radiochemical separation and ultra-sensitive mass spectrometric analysis of actinides2018

    • Author(s)
      Jian Zheng
    • Organizer
      Fukushima Research Conference on Development of Analytical Techniques in Waste management (FRCWM2018)
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Release of plutonium isotopes from the Fukushima Daiichi Nuclear Power Plant accident: distribution, source identification and dose estimation2018

    • Author(s)
      Jian Zheng
    • Organizer
      The 3rd Global Chinese Congress of Radiation Research, The Chinese Committee of the ICRP(招待講演)(国際学会)
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Simultaneous determination of ultra-trace level 237Np and Pu isotopes in soil/sediment samples by sector-field ICP-MS with a single-column chromatographic separation2018

    • Author(s)
      Zhaoya Huang, Youyi Ni, Hai Wang, Jian Zheng, Shigeo Uchida, Aya Sakaguchi
    • Organizer
      日本分析化学会第67年会, 日本分析化学会
    • Related Report
      2018 Research-status Report
  • [Presentation] Environmental dynamics of Pu isotopes released from the Fukushima nuclear accident2018

    • Author(s)
      Jian Zheng
    • Organizer
      Fukushima University, 4th Annual Report Symposium
    • Related Report
      2017 Research-status Report
    • Invited
  • [Presentation] Ultra-trace determination of Pu using SF-ICP-MS for a field study in Japan on soil to crop transfer of global fallout plutonium.2017

    • Author(s)
      Jian Zheng, Zhongtang Wang, Youyi Ni, Keiko Tagami, Shigeo Uchida
    • Organizer
      Asia-Pacific Winter Conference of Plasma Chemistry (APWC 2017), Matsue, Japan
    • Related Report
      2017 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Advance of mass spectrometric techniques for ultra-trace determination of radionuclides and its application in environmental radiochemistry2017

    • Author(s)
      Jian Zheng
    • Organizer
      Xinda Lecture, College of Chemistry and Engineering, Peking University, China
    • Related Report
      2017 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Radiochemical methods development and application based on the use of ICP-MS instruments2017

    • Author(s)
      Jian Zheng
    • Organizer
      Nordic Nuclear Safety Research, NKS-B ICP User Seminar, Denmark
    • Related Report
      2017 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Tracing the Fukushima nuclear accident released radiocesium and Pu isotopes in the environment: the role of isotope ratio analysis for nuclear forensics.2017

    • Author(s)
      Jian Zheng
    • Organizer
      Nuclear Emergency Expert Meeting (NEXT 2017), Hannover, Germany
    • Related Report
      2017 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Pu distributin in seawater and sediments in the Pacific off Fukushima after the FDNPP accident2017

    • Author(s)
      Jian Zheng, T. Aono, M. Yamada, K. Tagami, S. Uchida
    • Organizer
      Actinides 2017, Sendai, Japan
    • Related Report
      2017 Research-status Report
    • Int'l Joint Research
  • [Book] Chapter, 1.The Key Role of Isotopic Analysis in Tracing the Fukushima Nuclear Accident-Released Pu and Radiocesium Isotopes in the Environment. In Nuclear Emergencies. Current Topics in Environmental Health and Preventive Medicine2019

    • Author(s)
      Youyi Ni, Jian Zheng, Qiuju Guo, Hai Wan
    • Total Pages
      236
    • Publisher
      Nature Springer
    • Related Report
      2019 Annual Research Report

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Published: 2017-04-28   Modified: 2022-02-21  

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