文献类型：期刊文献

英文题名：Selective oxidation of emerging contaminants by high-valent cobalt (IV)-Oxo species: Constructing high-spin Co(III) sites in Fenton-like system

作者：Wan, Zihao[1];Xu, Minghao[1];Zhou, Liang[1,2];Zhang, Ya[3];Yang, Xuerui[1,2];Lin, Sen[1,2];Chovelon, Jean-Marc[4];Zhou, Lei[1,2]

机构：[1]East China Univ Sci & Technol, Sch Resources & Environm Engn, State Environm Protect Key Lab Environm Risk Asse, Shanghai 200237, Peoples R China;[2]Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200092, Peoples R China;[3]Minist Ecol & Environm, State Environm Protect Key Lab Soil Environm Mana, Nanjing Inst Environm Sci, Nanjing 210042, Peoples R China;[4]Univ Claude Bernard Lyon 1, Univ Lyon, CNRS, IRCELYON, F-69626 Villeurbanne, France

年份：2025

卷号：364

外文期刊名：APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY

收录：;EI(收录号：20244817418131);WOS:【SCI-EXPANDED(收录号:WOS:001371484300001)】；

基金：This work is financially supported by the National Natural Science Foundation of China (No. 22176059 & 22306064), The Fellowship of China Postdoctoral Science Foundation (2023M731085), The Natural Science Foundation of Shanghai (23ZR1417500), and the Fundamental Research Funds for the Central Universities.

语种：英文

外文关键词：Heterogeneous catalysis; Fenton-like oxidation; Layered double hydroxide; Jahn-teller effect; High-valent cobalt-Oxo species

摘要：In this study, a novel strategy for selectively generating Co(IV)=O species during peroxymonosulfate (PMS) activation was proposed, utilizing an optimized Co4Cu1-layered double hydroxide (LDH) material with low-coordination and high-spin-state Co sites. The incorporation of Cu(II), influenced by the Jahn-Teller effect, altered the geometry and coordination at Co(III) sites, optimizing the filling of Co 3d orbitals. The Co4Cu1-LDH/PMS system demonstrated exceptional catalytic activity for degrading emerging contaminants (ECs) across various water matrices, with a high concentration of Co(IV)=O generation. Continuous flow experiments showed an average 97.51 % degradation over 10 hours, indicating significant practical potential. Mechanistically, enhanced performance was attributed to a single electron transfer process and optimized orbital configurations for oxygen ligands at Co(III) sites. This study offers both theoretical insights and practical guidance for developing efficient catalysts targeting Co(IV)=O species in Fenton-like systems.