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Rapid Method To Determine 137Cs, 237Np, and Pu Isotopes in Seawater by SF-ICP-MS

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    Rapid Method To Determine 137Cs, 237Np, and Pu Isotopes in Seawater by SF-ICP-MS
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    • Shuai Zhang
      Shuai Zhang
      Institute of Radiological Sciences, National Institutes for Quantum Science and Technology, 4-9-1 Anagawa, Inage , Chiba 263-8555, Japan
      School of Geographic and Oceanographic Sciences, Nanjing University, Nanjing 210023, China
      More by Shuai Zhang
    • Zhiyong Liu
      Zhiyong Liu
      Institute of Radiological Sciences, National Institutes for Quantum Science and Technology, 4-9-1 Anagawa, Inage , Chiba 263-8555, Japan
      State Key Laboratory of Radiation Medicine and Protection, School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Centre of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University, Suzhou 215123, China
      More by Zhiyong Liu
      Orcidhttps://orcid.org/0000-0002-7665-2166
    • Guosheng Yang
      Guosheng Yang
      Institute of Radiological Sciences, National Institutes for Quantum Science and Technology, 4-9-1 Anagawa, Inage , Chiba 263-8555, Japan
      More by Guosheng Yang
      Orcidhttps://orcid.org/0000-0002-6478-249X
    • Jian Zheng*
      Jian Zheng
      Institute of Radiological Sciences, National Institutes for Quantum Science and Technology, 4-9-1 Anagawa, Inage , Chiba 263-8555, Japan
      *Email: [email protected]
      More by Jian Zheng
      Orcidhttps://orcid.org/0000-0003-0616-5570
    • Shaoming Pan*
      Shaoming Pan
      School of Geographic and Oceanographic Sciences, Nanjing University, Nanjing 210023, China
      *Email: [email protected]
      More by Shaoming Pan
    • Tatsuo Aono
      Tatsuo Aono
      Institute of Radiological Sciences, National Institutes for Quantum Science and Technology, 4-9-1 Anagawa, Inage , Chiba 263-8555, Japan
      Radioecology Unit, Fukushima Institute for Research, Education and Innovation, 1 Hikariga-oka, Fukushima, Fukushima 960-1295, Japan
      More by Tatsuo Aono
    • Aya Sakaguchi
      Aya Sakaguchi
      Institute of Pure and Applied Sciences, University of Tsukuba, 1-1-1 Tennodai, Tsukuba , Ibaraki 305-8577, Japan
      More by Aya Sakaguchi
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    Analytical Chemistry

    Cite this: Anal. Chem. 2023, 95, 46, 16892–16901
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    https://doi.org/10.1021/acs.analchem.3c02702
    Published October 31, 2023
    Copyright © 2023 American Chemical Society
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    Abstract

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    Neptunium-237, owing to its long half-life (t1/2 = 2.14 × 106 year) and similar conservatism to 137Cs, has the potential to replace 137Cs for water mass circulation studies on decades and even longer time scales. A new method for the determination of 137Cs, 237Np, and Pu isotopes in seawater samples was proposed to solve the difficulty of 237Np analysis in seawater. The developed method includes the separation technique of ammonium phosphomolybdate (AMP) adsorption for 137Cs and anion exchange chromatography for 237Np and Pu, a measurement technique of gamma spectrometry for 137Cs and SF-ICP-MS for 237Np and Pu isotopes. 242Pu as a pseudo isotope dilution tracer for Np, the negligible chemical fractionation between 237Np and 242Pu of 1.02 ± 0.06 (k = 2) was obtained by implementing sophisticated control of the redox system and chromatographic elution optimization. The analytical results for the International Atomic Energy Agency Certified Reference Materials (IAEA-443) agreed with the reference values, showing chemical yields of 65–88%, U decontamination factor above 106 level, and improved sample throughput (5 days for 12 samples). Meanwhile, the lower method detection limits (MDLs) of 237Np, 239Pu, and 240Pu were 1.3 × 10–3, 0.065, and 0.15 μBq L–1 for 15 L seawater, respectively. Results obtained by the developed method can be used to evaluate the impact on the marine ecological system of the planned marine discharge of Fukushima decontaminated wastewater. Working toward that purpose, we are the first to report the 237Np activity concentration in Pacific Ocean seawater sampled near the station site, and we obtained the value of 0.122–0.154 μBq L–1.

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.analchem.3c02702.

    • Optimization results of CaF2/LaF3 coprecipitation; simulated seawater preparation; statistical analyses of 237Np data for reference materials; comparison of 237Np and Pu isotopes MDLs; and reagents and materials (PDF)

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    Cited By

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    This article is cited by 5 publications.

    1. Xiang Gu, Bo Yang, Guosheng Yang, Masatoshi Yamada, Fengchang Wu, Jian Zheng. Determination of ultra-trace Pu isotopes in large-volume seawater samples from the South Pacific Ocean using sector field ICP-MS combined with extraction chromatography. Microchemical Journal 2025, 208 , 112480. https://doi.org/10.1016/j.microc.2024.112480
    2. S. Mialle, A. Nonell, C. Cruchet, C. Caussignac, M. Marie, A. Rincel, H. Isnard. Direct determination of the 237Np/238U ratio in nuclear fuel samples by multicollection inductively coupled plasma mass spectrometry (MC-ICP-MS). Journal of Radioanalytical and Nuclear Chemistry 2024, 333 (10) , 4825-4835. https://doi.org/10.1007/s10967-024-09659-4
    3. Bo Yang, Jian Zheng, Guosheng Yang, Ning Qin, Keiko Tagami, Shigeo Uchida. Characterization of typical transuranic nuclides in a reference fallout material using SF-ICP-MS. Journal of Environmental Radioactivity 2024, 278 , 107506. https://doi.org/10.1016/j.jenvrad.2024.107506
    4. Alexandre Quemet, Amélie Hubert, Alkiviadis Gourgiotis, Ana María Sánchez Hernández, Marielle Crozet, Guillaume Bailly, Andrew Dobney, Georges Duhamel, Joe Hiess, Urska Repinc, Sébastien Mialle, Béatrice Boulet, Raphaëlle Escoube, Céline Bouvier-Capely, Fabien Pointurier, Sébastien Picart. An isotope dilution mass spectrometry overview: tips and applications for the measurement of radionuclides. Journal of Analytical Atomic Spectrometry 2024, 39 (7) , 1665-1699. https://doi.org/10.1039/D4JA00029C
    5. Ning Qin, Jian Zheng, Guosheng Yang, Keiko Tagami. A comprehensive survey of reference materials for their use in quality assurance for the determination of Np-237 in environmental samples. Journal of Environmental Radioactivity 2024, 271 , 107328. https://doi.org/10.1016/j.jenvrad.2023.107328
    6. Bo Yang, Jian Zheng, Guosheng Yang, Ning Qin, Keiko Tagami, Shigeo Uchida. Characterization of Typical Transuranic Nuclides in a Reference Fallout Material Using Sf-Icp-Ms. 2024https://doi.org/10.2139/ssrn.4836808
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    Analytical Chemistry

    Cite this: Anal. Chem. 2023, 95, 46, 16892–16901
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.analchem.3c02702
    Published October 31, 2023
    Copyright © 2023 American Chemical Society
    Request reuse permissions

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