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

Ming-Yan Lan, Yu-Hang Li, Chong-Chen Wang (), Xin-Jie Li, Jiazhen Cao, Linghui Meng, Shuai Gao, Yuhui Ma, Haodong Ji () and Mingyang Xing ()
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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

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-51525-0

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