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Exploring the Reduction Mechanism of 99Tc(VII) in NaClO4: A Spectro-Electrochemical Approach

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    Exploring the Reduction Mechanism of 99Tc(VII) in NaClO4: A Spectro-Electrochemical Approach
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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2022, 61, 26, 10159–10166
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    https://doi.org/10.1021/acs.inorgchem.2c01278
    Published June 24, 2022
    Copyright © 2022 American Chemical Society
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    Abstract

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    Technetium (Tc) is an environmentally relevant radioactive contaminant whose migration is limited when Tc(VII) is reduced to Tc(IV). However, its reaction mechanisms are not well understood yet. We have combined electrochemistry, spectroscopy, and microscopy (cyclic voltammetry, rotating disk electrode, X-ray photoelectron spectroscopy, and Raman and scanning electron microscopy) to study Tc(VII) reduction in non-complexing media: 0.5 mM KTcO4 in 2 M NaClO4 in the pH from 2.0 to 10.0. At pH 2.0, Tc(VII) first gains 2.3 ± 0.3 electrons, following Tc(V) rapidly receives 1.3 ± 0.3 electrons yielding Tc(IV). At pH 4.0–10.0, Tc(IV) is directly obtained by transfer of 3.2 ± 0.3 electrons. The reduction of Tc(VII) produced always a black solid identified as Tc(IV) by Raman and XPS. Our results narrow a significant gap in the fundamental knowledge of Tc aqueous chemistry and are important to understand Tc speciation. They provide basic steps on the way from non-complexing to complex media.

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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.inorgchem.2c01278.

    • In-house built spectro-electrochemical cell; reduction curves; CVs at different scan rates; and SEM–EDX experimental description of Tc solid analysis (PDF)

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    This article is cited by 4 publications.

    1. Erik Strub, Désirée Badea, Jörn Bruns, Antonio Frontera, Natalia Mayordomo, Anna Sakhonenkova, Maximilian Roca Jungfer, Mathias Wickleder, Clarence Yong, Markus Zegke. Technetium ‐ The Unknown Center of the Periodic Table. European Journal of Inorganic Chemistry 2025, https://doi.org/10.1002/ejic.202400780
    2. Ting Yu, Hu Zhang, Yongzhi Ning, Hongling Li, Ziteng Gao, Bo Wang, Zhijun Cen. Experimental and Kinetic Simulations of Technetium-Catalyzed Hydrazine Oxidation in Nitric Acid Solution. Processes 2024, 12 (11) , 2319. https://doi.org/10.3390/pr12112319
    3. Ruijie Li, Yun Gong, Jianhua Lin. NaSbF4 nanoparticles as solid-state electrolytes in sodium-iodine batteries: sodium ion transport via conversion reaction and shuttle effect retarded by fluoride. Journal of Power Sources 2024, 602 , 234352. https://doi.org/10.1016/j.jpowsour.2024.234352
    4. Guillaume Delaittre, Georg Dierkes, Johanna Heine, Constantin Hoch, Ullrich Jahn, Hajo Kries, Björn Meermann, Erik Strub, Carl Christoph Tzschucke. Notizen aus der Chemie. Nachrichten aus der Chemie 2023, 71 (2) , 42-45. https://doi.org/10.1002/nadc.20234134634
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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2022, 61, 26, 10159–10166
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.inorgchem.2c01278
    Published June 24, 2022
    Copyright © 2022 American Chemical Society
    Request reuse permissions

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