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Artificial Photosynthetic Assemblies Constructed by NH2-UiO-66 Decorated with Spatially Separated Dual Cocatalysts for Enhanced Photocatalytic Uranium Reduction
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    Artificial Photosynthetic Assemblies Constructed by NH2-UiO-66 Decorated with Spatially Separated Dual Cocatalysts for Enhanced Photocatalytic Uranium Reduction
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    • Xudong Wu
      Xudong Wu
      State Key Laboratory of Environment-friendly Energy Materials, National Co-innovation Center for Nuclear Waste Disposal and Environmental Safety, Sichuan Civil-military Integration Institute, School of National Defence & Technology, School of Materials and Chemistry, Southwest University of Science and Technology, Mianyang, Sichuan 621010, P. R. China
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    • Kaifu Yu
      Kaifu Yu
      State Key Laboratory of Environment-friendly Energy Materials, National Co-innovation Center for Nuclear Waste Disposal and Environmental Safety, Sichuan Civil-military Integration Institute, School of National Defence & Technology, School of Materials and Chemistry, Southwest University of Science and Technology, Mianyang, Sichuan 621010, P. R. China
      College of Chemistry, Key Laboratory of Radiation Physics & Technology, Ministry of Education, Sichuan University, Chengdu, Sichuan 610064, P. R. China
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    • Yizhou He
      Yizhou He
      State Key Laboratory of Environment-friendly Energy Materials, National Co-innovation Center for Nuclear Waste Disposal and Environmental Safety, Sichuan Civil-military Integration Institute, School of National Defence & Technology, School of Materials and Chemistry, Southwest University of Science and Technology, Mianyang, Sichuan 621010, P. R. China
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    • Xin Cao
      Xin Cao
      State Key Laboratory of Environment-friendly Energy Materials, National Co-innovation Center for Nuclear Waste Disposal and Environmental Safety, Sichuan Civil-military Integration Institute, School of National Defence & Technology, School of Materials and Chemistry, Southwest University of Science and Technology, Mianyang, Sichuan 621010, P. R. China
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    • Tao Chen*
      Tao Chen
      State Key Laboratory of Environment-friendly Energy Materials, National Co-innovation Center for Nuclear Waste Disposal and Environmental Safety, Sichuan Civil-military Integration Institute, School of National Defence & Technology, School of Materials and Chemistry, Southwest University of Science and Technology, Mianyang, Sichuan 621010, P. R. China
      *Email: [email protected]
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    • Wenkun Zhu*
      Wenkun Zhu
      State Key Laboratory of Environment-friendly Energy Materials, National Co-innovation Center for Nuclear Waste Disposal and Environmental Safety, Sichuan Civil-military Integration Institute, School of National Defence & Technology, School of Materials and Chemistry, Southwest University of Science and Technology, Mianyang, Sichuan 621010, P. R. China
      *Email: [email protected]
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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2024, 63, 51, 24141–24149
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    https://doi.org/10.1021/acs.inorgchem.4c03786
    Published December 11, 2024
    Copyright © 2024 American Chemical Society

    Abstract

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    The phenomenon of rapid migration of photogenerated charges in natural photosynthetic systems has motivated the design of efficient photocatalysts capable of fast charge separation and efficient reaction kinetics for photocatalytically assisted enrichment and separation of uranium U(VI) in uranium wastewater. In this study, we developed a biomimetic photocatalytic system MnOx/NH2-UiO-66-rGO (M/UiO-rGO) with spatially separated dual cocatalysts. Among them, rGO functions to capture electrons and participates in reduction reactions, while MnOx captures holes and participates in oxidation reactions. The M/UiO-rGO catalyst exhibits excellent performance in photocatalytic reduction of uranium (reaching 91.8% in 1 h), and even under natural light conditions, it exhibits excellent uranium removal ability (80.4%). Using multispectral coupling technology, we further confirmed that enriched uranium undergoes a continuous and complex reaction process of “capture-reduction-free radical oxidation–nucleation–crystallization”. This work presents a viable strategy for designing biomimetic photocatalysts with efficient charge separation and rapid reaction kinetics for environmental purification purposes.

    Copyright © 2024 American Chemical Society

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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.4c03786.

    • Additional experimental details, related structural figures, SEM images, EDS analysis, TG curve, PXRD, ζ potential curves, UPS valence-band curves, and electrochemical curves (PDF)

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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2024, 63, 51, 24141–24149
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.inorgchem.4c03786
    Published December 11, 2024
    Copyright © 2024 American Chemical Society

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