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Secondary metal ion-induced electrochemical reduction of U(VI) to U(IV) solids

Author

Listed:
  • Xiaolu Liu

    (North China Electric Power University
    University of North Texas)

  • Yinghui Xie

    (North China Electric Power University)

  • Mengjie Hao

    (North China Electric Power University)

  • Yang Li

    (North China Electric Power University)

  • Zhongshan Chen

    (North China Electric Power University)

  • Hui Yang

    (North China Electric Power University)

  • Geoffrey I. N. Waterhouse

    (The University of Auckland)

  • Xiangke Wang

    (North China Electric Power University)

  • Shengqian Ma

    (University of North Texas)

Abstract

Recent studies have shown that aqueous U(VI) ions can be transformed into U(VI) precipitates through electrocatalytic redox reactions for uranium recovery. However, there have been no reports of U(IV) solids, such as UO2, using electrochemical methods under ambient conditions since low-valence states of uranium are typically oxidized to U(VI) by O2 or H2O2. Here we developed a secondary metal ion-induced strategy for electrocatalytic production of U(IV) solids from U(VI) solutions using a catalyst consisting of atomically dispersed gallium on hollow nitrogen-doped carbon capsules (Ga-Nx-C). This method relies on the presence of secondary metal ions, e.g., alkaline earth metals, transition metals, lanthanide metals, and actinide metals, which promote the generation of UO2 or bimetallic U(IV)-containing oxides through a two-electron transfer process. No U(IV) solid products were generated in the presence of alkali metal ions. Mechanistic studies revealed that the strong binding affinity between U(IV) and alkaline earth metals (Ca2+/Mg2+/Sr2+/Ba2+), transition metals (Ni2+/Zn2+/Pb2+/Fe3+, etc.) and lanthanide/actinide metals (Ce4+/Eu3+/Th4+/La3+) suppressed re-oxidation of U(IV) to U(VI), leading to the generation of U(IV)O2 and Mx(M = Ce, Eu, Th, La)U(IV)yO2. This work provides fundamental insights into the electrochemical behavior of uranium in aqueous media, whilst guiding uranyl capture from nuclear waste and contaminated water.

Suggested Citation

  • Xiaolu Liu & Yinghui Xie & Mengjie Hao & Yang Li & Zhongshan Chen & Hui Yang & Geoffrey I. N. Waterhouse & Xiangke Wang & Shengqian Ma, 2024. "Secondary metal ion-induced electrochemical reduction of U(VI) to U(IV) solids," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-52083-1
    DOI: 10.1038/s41467-024-52083-1
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    References listed on IDEAS

    as
    1. Yihui Yuan & Qiuhan Yu & Meng Cao & Lijuan Feng & Shiwei Feng & Tingting Liu & Tiantian Feng & Bingjie Yan & Zhanhu Guo & Ning Wang, 2021. "Selective extraction of uranium from seawater with biofouling-resistant polymeric peptide," Nature Sustainability, Nature, vol. 4(8), pages 708-714, August.
    2. Zezhen Pan & Barbora Bártová & Thomas LaGrange & Sergei M. Butorin & Neil C. Hyatt & Martin C. Stennett & Kristina O. Kvashnina & Rizlan Bernier-Latmani, 2020. "Nanoscale mechanism of UO2 formation through uranium reduction by magnetite," Nature Communications, Nature, vol. 11(1), pages 1-12, December.
    3. Vladislav A. Petrov & Michael I. Ojovan & Sergey V. Yudintsev, 2023. "Material Aspect of Sustainable Nuclear Waste Management," Sustainability, MDPI, vol. 15(15), pages 1-7, August.
    4. Zhongshan Chen & Jingyi Wang & Mengjie Hao & Yinghui Xie & Xiaolu Liu & Hui Yang & Geoffrey I. N. Waterhouse & Xiangke Wang & Shengqian Ma, 2023. "Tuning excited state electronic structure and charge transport in covalent organic frameworks for enhanced photocatalytic performance," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
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