文献类型：期刊文献

英文题名：Coupling-promoted oxidative degradation of organic micropollutants by iron oxychloride (FeOCl) with dual active sites

作者：Wang, Jinling[1,2];Zhong, Shifa[3];Wen, Yuzhen[1];Li, Jianan[1];Wang, Hualin[1,2];Liu, Honglai[2];Cui, Changzheng[1];Gong, Ming[4,5];Zhang, Huichun[3];Yang, Xuejing[1,2]

机构：[1]East China Univ Sci & Technol ECUST, Natl Engn Lab Ind Wastewater Treatment, Shanghai 200237, Peoples R China;[2]ECUST, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[3]Case Western Reserve Univ, Dept Civil Engn, 2104 Adelbert Rd, Cleveland, OH 44106 USA;[4]Fudan Univ, Dept Chem, Shanghai 200438, Peoples R China;[5]Fudan Univ, Shanghai Key Lab Mol Catalysis & Innovat Mat, Shanghai 200438, Peoples R China

年份：2022

卷号：9

外文期刊名：CHEMICAL ENGINEERING JOURNAL ADVANCES

收录：WOS:【ESCI(收录号:WOS:001112797300002)】；

基金：The authors acknowledge the was supported financially by National Key Basic Research Program of China (2019YFA0705800, 2019YFC1906700) , the National Natural Science Foundation of China (No. 22006039, 21876049 and 91834301) , the Strategic Priority Research Program of the Chinese Academy of Sciences (XDA23010400) and the China Postdoctoral Science Foundation (2019M661412) .

语种：英文

外文关键词：FeOCl; Fenton chemistry; Ferryl-oxo; Micropollutants; Oxidative coupling

摘要：Heterogeneous Fenton has emerged as a profitable solution for contaminant removal via advanced oxidation processes (AOPs). Besides the dominant hydroxyl radicals (HO center dot), some weaker oxidants, such as ferryl-oxo species (Fe(IV)=O) species, can also be produced during the surface H2O2 activation, but its function is not well understood. In this study, we developed a vanadium-etched iron oxychloride (V-FeOCl) catalyst that simultaneously incorporates Fenton-like sites and peroxidase-like (Fe(IV)=O) sites. The derived V-FeOCl material showed 2.8-5.4 times enhancement of the pseudo-first-order rate constant for various recalcitrant organic micropollutants. Most importantly, the activity demonstrated an intriguing induction period for the TOC removal as well as a rocketed kinetics after the induction. This induction period was further attributed to the oxidative coupling of the organic monomers, as revealed by the identification of dimers using UPLC-MS. The coupling intermediates were demonstrated to be more susceptible to HO center dot radical attack via the high-throughput prediction of the HO center dot radical rate constants of 94 possible coupling intermediates using machine learning. These findings clarified the key role of Fe(IV)=O in the HO center dot-based oxidation process and points to a novel couplingenhanced degradation pathway, which could potentially pave a new avenue of oxidative transformations for catalytic and environmental applications.