文献类型：期刊文献

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

作者：Lan, Ming-Yan[1];Li, Yu-Hang[2];Wang, Chong-Chen[1];Li, Xin-Jie[1];Cao, Jiazhen[3];Meng, Linghui[1];Gao, Shuai[2];Ma, Yuhui[4];Ji, Haodong[2];Xing, Mingyang[3]

机构：[1]Beijing Univ Civil Engn & Architecture, Sch Environm & Energy Engn, Beijing Key Lab Funct Mat Bldg Struct & Environm, Beijing, Peoples R China;[2]Peking Univ, Shenzhen Grad Sch, Sch Environm & Energy, Ecoenvironm & Resource Efficiency Res Lab, Shenzhen, Guangdong, Peoples R China;[3]East China Univ Sci & Technol, Sch Resources & Environm Engn, Natl Engn Res Ctr Ind Wastewater Detoxicat & Reso, Shanghai, Peoples R China;[4]Chinese Acad Sci, Inst High Energy Phys, Key Lab Biomed Effects Nanomat & Nanosafety, Beijing, Peoples R China

年份：2024

卷号：15

期号：1

外文期刊名：NATURE COMMUNICATIONS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:001371634200010)】；

基金：This work was supported by National Natural Science Foundation of China (22176012, 52370025, 52100069, 22325602, 12175263, 22176060), the Cultivation project Funds for Beijing University of Civil Engineering and Architecture (X23034) and the Shenzhen Science and Technology Program (JCYJ20220531093205013), and the Program of Shanghai Academic/Technology Research Leader (23XD1421000).

语种：英文

摘要：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, Co-2(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, Co-2(V4O12)(bpy)(2) exhibits long-term water purification ability, up to 40h, 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.