文献类型：期刊文献

英文题名：Oxygen Vacancies Engineering of Co3O4 to Modulate the Adjacent Environment: Boosted Singlet Oxygen Generation in Peroxymonosulfate-Mediated 2-Chlorophenol Degradation

作者：Wang, Feng[1];Zhou, Yilong[1];Weng, Xiaole[2];Wang, Li[1];Gao, Shan[3];Zhao, Yemin[3];Zhan, Wangcheng[1];Guo, Yanglong[1];Dai, Qiguang[1]

机构：[1]East China Univ Sci & Technol, Res Inst Ind Catalysis, Sch Chem & Mol Engn, State Key Lab Green Chem Engn & Ind Catalysis, Shanghai 200237, Peoples R China;[2]Zhejiang Univ, Coll Environm & Resource Sci, Key Lab Environm Remediat & Ecol Hlth, Minist Educ, Hangzhou 310058, Peoples R China;[3]Zhejiang Tianlan Environm Protect Technol Co Ltd, Hangzhou 311202, Peoples R China

年份：2025

卷号：59

期号：38

起止页码：20792

外文期刊名：ENVIRONMENTAL SCIENCE & TECHNOLOGY

收录：;EI(收录号：20254019259843);WOS:【SCI-EXPANDED(收录号:WOS:001575405800001)】；

基金：This work was supported by the National Key Research and Development Program of China (2023YFC3707500 and 2022YFB3504200) and the National Natural Science Foundation of China (22276055 and 21922602). The authors thank Research Center of Analysis and Test of East China University of Science and Technology for the help on the characterization.

语种：英文

外文关键词：peroxymonosulfate activation; singlet oxygen; oxygen vacancies; adjacent heteronucleardiatomic sites; oxygen vacancies anchoring

摘要：Peroxymonosulfate-based advanced oxidation processes are promising for removing organic pollutants but precisely generating singlet oxygen (O-1(2)) as nonradical reactive oxygen species is difficult. Herein, a porous Co3O4 nanosheet was synthesized and further tailored by the bulk doping of Mn and the surface loading of Ru. The abundant oxygen vacancies (Ov) could be created by the Mn doping and then facilitated the precise anchoring of Ru, which in turn contributed to the construction of the adjacent heteronuclear diatomic adsorbed sites (Co-Ov-Ru). In the base MnCoO x /peroxymonosulfate (PMS) system, the electron transfer occurred between the Co(III)-(O)OSO3- complex and free HSO5- to produce the O-2(center dot-) and subsequently the adjacent O-2(center dot-) trapped on the Ov disproportionates into O-1(2), whereas the anchoring of Ru occupied the Ov and high-selectively boosted the self-combined generation of O-1(2) through the heteronuclear diatomic-adsorbed PMS (SO5 center dot--Co-Ov-Ru-SO5 center dot-). The optimized Ru/MnCoO x demonstrated wide pH adaptability, high efficiency, and salinity tolerance for the degradation of 2-chlorophenol, and it removes over 99% of contaminants in complex water matrices even after 36 h in fixed-bed operation. This work provided a new protocol for PMS activation through a distinctively structured and easily scaled Co3O4-based catalyst and contributed to understand the tuning generation of singlet oxygen and guide the design of metal oxide catalysts.