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Ultratrace Determination of 99Tc in Small Natural Water Samples by Accelerator Mass Spectrometry with the Gas-Filled Analyzing Magnet System

  • Francesca Quinto*
    Francesca Quinto
    Institute for Nuclear Waste Disposal, Karlsruhe Institute of Technology, Hermann-von-Helmholtz-Platz 1, Eggenstein-Leopoldshafen D-76344, Germany
    *Phone: +49 721 608-22233. Fax: +49 721 608-23927. E-mail: [email protected]
  • Christoph Busser
    Christoph Busser
    Physik Department, Technische Universität München, James-Franck-Straße 1, Garching D-85748, Germany
  • Thomas Faestermann
    Thomas Faestermann
    Physik Department, Technische Universität München, James-Franck-Straße 1, Garching D-85748, Germany
  • Karin Hain
    Karin Hain
    VERA Laboratory, Faculty of Physics, University of Vienna, Währinger Straße 17, Vienna A-1090, Austria
    More by Karin Hain
  • Dominik Koll
    Dominik Koll
    Physik Department, Technische Universität München, James-Franck-Straße 1, Garching D-85748, Germany
    Department of Nuclear Physics, Research School of Physics and Engineering, The Australian National University, ACT, Canberra 2601, Australia
    More by Dominik Koll
  • Gunther Korschinek
    Gunther Korschinek
    Physik Department, Technische Universität München, James-Franck-Straße 1, Garching D-85748, Germany
  • Stephanie Kraft
    Stephanie Kraft
    Institute for Nuclear Waste Disposal, Karlsruhe Institute of Technology, Hermann-von-Helmholtz-Platz 1, Eggenstein-Leopoldshafen D-76344, Germany
  • Peter Ludwig
    Peter Ludwig
    Physik Department, Technische Universität München, James-Franck-Straße 1, Garching D-85748, Germany
    TÜV SÜD Industrie Service GmbH, Westendstraße 199, München D-80686, Germany
    More by Peter Ludwig
  • Markus Plaschke
    Markus Plaschke
    Institute for Nuclear Waste Disposal, Karlsruhe Institute of Technology, Hermann-von-Helmholtz-Platz 1, Eggenstein-Leopoldshafen D-76344, Germany
  • Thorsten Schäfer
    Thorsten Schäfer
    Institute for Nuclear Waste Disposal, Karlsruhe Institute of Technology, Hermann-von-Helmholtz-Platz 1, Eggenstein-Leopoldshafen D-76344, Germany
    Applied Geology, Institute for Geoscience, Friedrich-Schiller-University Jena, Burgweg 11, Jena D-07749, Germany
  • , and 
  • Horst Geckeis
    Horst Geckeis
    Institute for Nuclear Waste Disposal, Karlsruhe Institute of Technology, Hermann-von-Helmholtz-Platz 1, Eggenstein-Leopoldshafen D-76344, Germany
Cite this: Anal. Chem. 2019, 91, 7, 4585–4591
Publication Date (Web):March 7, 2019
https://doi.org/10.1021/acs.analchem.8b05765
Copyright © 2019 American Chemical Society

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    Abstract

    Abstract Image

    In the frame of studies on the safe disposal of nuclear waste, there is a great interest for understanding the migration behavior of 99Tc. 99Tc originating from nuclear energy production and global fallout shows environmental levels down to 107 atoms/g of soil (∼2 fg/g). Extremely low concentrations are also expected in groundwater after diffusion of 99Tc through the bentonite constituting the technical barrier for nuclear waste disposal. The main limitation to the sensitivity of the mass spectrometric analysis of 99Tc is the background of its stable isobar 99Ru. For ultratrace analysis, the Accelerator Mass Spectrometry (AMS) setup of the Technical University of Munich using a Gas-Filled Analyzing Magnet System (GAMS) and a 14 MV Tandem accelerator is greatly effective in suppressing this interference. In the present study, the GAMS setup is used for the analysis of 99Tc in samples of the seawater reference material IAEA-443, a peat bog lake, and groundwater from an experiment of in situ diffusion through bentonite in the controlled zone of the Grimsel Test Site (GTS) within the Colloid Formation and Migration (CFM) project. With an adapted chemical preparation procedure, measurements of 99Tc concentrations at the fg/g levels with a sensitivity down to 0.5 fg are accomplished in notably small natural water samples. The access to these low concentration levels allows for the long-term monitoring of in situ tracer tests over several years and for the determination of environmental levels of 99Tc in small samples.

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    Cited By

    This article is cited by 10 publications.

    1. Walter Kutschera, A. J. Timothy Jull, Michael Paul, Anton Wallner. Atom counting with accelerator mass spectrometry. Reviews of Modern Physics 2023, 95 (3) https://doi.org/10.1103/RevModPhys.95.035006
    2. Yun-Chong Fu, Lu-Yuan Zhang, Yan-Ting Bi, Qi Liu, Peng Cheng. Study of 99Tc and 129I measurement using 3MV Xi’an-AMS. Journal of Radioanalytical and Nuclear Chemistry 2023, 332 (4) , 1253-1261. https://doi.org/10.1007/s10967-022-08757-5
    3. M. Alam, Zinnat Begum, Yoshiaki Furusho, Hyoe Takata, Ismail Rahman. Study on Separation of Rhenium, a Surrogate Element of Fissiogenic Technetium, from Aqueous Matrices Using Ion-Selective Extraction Chromatographic Resins. Separations 2023, 10 (3) , 216. https://doi.org/10.3390/separations10030216
    4. Karin Hain, Stephanie Adler, Fadime Gülce, Martin Martschini, Johanna Pitters, Robin Golser. Isobar suppression studies for 99Tc detection using Ion-Laser InterAction Mass Spectrometry (ILIAMS). Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms 2022, 531 , 109-114. https://doi.org/10.1016/j.nimb.2022.09.016
    5. Wenting Bu, Liang Yang, Lei Tang, Ke Xiong, Youyi Ni, Chuting Yang, Sheng Hu. Eliminating Mo isobaric interference using O 2 as reaction gas for Tc measurement by triple quadrupole ICP-MS. Journal of Analytical Atomic Spectrometry 2022, 37 (6) , 1174-1178. https://doi.org/10.1039/D2JA00104G
    6. Karin Hain, Martin Martschini, Fadime Gülce, Maki Honda, Johannes Lachner, Michael Kern, Johanna Pitters, Francesca Quinto, Aya Sakaguchi, Peter Steier, Andreas Wiederin, Alexander Wieser, Akihiko Yokoyama, Robin Golser. Developing Accelerator Mass Spectrometry Capabilities for Anthropogenic Radionuclide Analysis to Extend the Set of Oceanographic Tracers. Frontiers in Marine Science 2022, 9 https://doi.org/10.3389/fmars.2022.837515
    7. Vanessa Montoya, Ulrich Noseck, Felix Mattick, Susan Britz, Ingo Blechschmidt, Thorsten Schäfer. Radionuclide geochemistry evolution in the Long-term In-situ Test (LIT) at Grimsel Test Site (Switzerland). Journal of Hazardous Materials 2022, 424 , 127733. https://doi.org/10.1016/j.jhazmat.2021.127733
    8. Mercedes López-Lora, Elena Chamizo, Isabelle Levy, Marcus Christl, Núria Casacuberta, Timothy C. Kenna. 236U, 237Np and 239,240Pu as complementary fingerprints of radioactiveeffluents in the western Mediterranean Sea and in the Canada Basin (Arctic Ocean). Science of The Total Environment 2021, 765 , 142741. https://doi.org/10.1016/j.scitotenv.2020.142741
    9. Lei Tang, Wenting Bu, Xuemei Liu, Sheng Hu. More than ten percent ionization efficiency for Tc measurement by negative thermal ionization mass spectrometry. Journal of Analytical Atomic Spectrometry 2019, 34 (11) , 2229-2235. https://doi.org/10.1039/C9JA00291J
    10. Simon Carter, Robert Clough, Andy Fisher, Bridget Gibson, Ben Russell, Julia Waack. Atomic spectrometry update: review of advances in the analysis of metals, chemicals and materials. Journal of Analytical Atomic Spectrometry 2019, 34 (11) , 2159-2216. https://doi.org/10.1039/C9JA90058F

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