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Multi-channel electron transfer induced by polyvanadate in metal-organic framework for boosted peroxymonosulfate activation

Author

Listed:
  • Ming-Yan Lan

    (Beijing University of Civil Engineering and Architecture)

  • Yu-Hang Li

    (Peking University Shenzhen Graduate School)

  • Chong-Chen Wang

    (Beijing University of Civil Engineering and Architecture)

  • Xin-Jie Li

    (Beijing University of Civil Engineering and Architecture)

  • Jiazhen Cao

    (East China University of Science and Technology)

  • Linghui Meng

    (Beijing University of Civil Engineering and Architecture)

  • Shuai Gao

    (Peking University Shenzhen Graduate School)

  • Yuhui Ma

    (Chinese Academy of Sciences)

  • Haodong Ji

    (Peking University Shenzhen Graduate School)

  • Mingyang Xing

    (East China University of Science and Technology)

Abstract

Catalytic peroxymonosulfate (PMS) activation processes don’t solely rely on electron transfer from dominant metal centers due to the complicated composition and interface environment of catalysts. Herein the synthesis of a cobalt based metal-organic framework containing polyvanadate [V4O12]4− cluster, Co2(V4O12)(bpy)2 (bpy = 4,4’-bipyridine), is presented. The catalyst demonstrates superior degradation activity toward various micropollutants, with higher highest occupied molecular orbital (HOMO), via nonradical attack. The X-ray absorption spectroscopy and density functional theory (DFT) calculations demonstrate that Co sites act as both PMS trapper and electron donor. In situ spectral characterizations and DFT calculations reveal that the terminal oxygen atoms in the [V4O12]4− electron sponge could interact with the terminal hydrogen atoms in PMS to form hydrogen bonds, promoting the generation of SO5* intermediate via both dynamic pull and direct electron transfer process. Further, Co2(V4O12)(bpy)2 exhibits long-term water purification ability, up to 40 h, towards actual wastewater discharged from an ofloxacin production factory. This work not only presents an efficient catalyst with an electron sponge for water environmental remediation via nonradical pathway, but also provides fundamental insights into the Fenton-like reaction mechanism.

Suggested Citation

  • Ming-Yan Lan & Yu-Hang Li & Chong-Chen Wang & Xin-Jie Li & Jiazhen Cao & Linghui Meng & Shuai Gao & Yuhui Ma & Haodong Ji & Mingyang Xing, 2024. "Multi-channel electron transfer induced by polyvanadate in metal-organic framework for boosted peroxymonosulfate activation," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-51525-0
    DOI: 10.1038/s41467-024-51525-0
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    References listed on IDEAS

    as
    1. Dongpeng Zhang & Yanxiao Li & Pengfei Wang & Jinyong Qu & Yi Li & Sihui Zhan, 2023. "Dynamic active-site induced by host-guest interactions boost the Fenton-like reaction for organic wastewater treatment," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
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