文献类型：期刊文献

英文题名：Ferryl-Involved Oxidation Coupling Processes over K x FeOCl Enzyme-Mimetic Catalysis: Mechanistic Insights and Kinetic Modeling

作者：Wang, Yongjie[1,2];Xu, Shengshuo[1,2];Wang, Jinling[1];Duan, Yanghua[3];Qian, Yuanyuan[2,4];Wang, Hualin[1];Xu, Yanjing[2,4];Yang, Xuejing[1,2]

机构：[1]East China Univ Sci & Technol, Natl Engn Lab Ind Wastewater Treatment, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Shanghai Engn Lab Lean Operat Technol Ind Water Sy, Shanghai 200237, Peoples R China;[3]Univ Calif Berkeley, Dept Civil & Environm Engn, Berkeley, CA 94720 USA;[4]McWong Environm Technol Co Ltd, Shanghai 200135, Peoples R China

年份：2023

卷号：3

期号：9

起止页码：2978

外文期刊名：ACS ES&T WATER

收录：WOS:【ESCI(收录号:WOS:001031738700001)】；

基金：This work was supported financially by grants from the National Key Research and Development Program of China (2019YFA0705800), National Natural Science Foundation of China (21876049 and 22222602), Shanghai Technology Innovation Program of Technical Center (20DZ2250600), and Shanghai Pujiang Program (21PJD016).

语种：英文

外文关键词：oxidative coupling; kinetics; intercalation; enzyme-mimetic system; environmental pollution

摘要：Enzyme-mimetic metal-based catalysts have received extensiveattentionfor the efficient catalytic applications. These catalysts can be adaptedto complex environmental circumstances, thus becoming one of the effectiveways to deal with refractory pollutants. In previous research, theK(+)-intercalated FeOCl (K x FeOCl)catalyst can produce Fe(IV)O intermediate species throughheterocleavage of H2O2 in a similar way as naturalperoxidases. In this study, the detailed kinetics and surface reactionmechanisms of K x FeOCl were comprehensivelyinvestigated using 2-methoxyphenol (2-MeOP) as the model contaminantand at pH 7. 2-MeOP molecules are oxidized to organic radicals, whichfurther oxidize 2-MeOP for direct radical-radical coupling.Based on the kinetics, the Langmuir-Hinshelwood model was usedto describe the oxidative coupling of 2-MeOP on the K x FeOCl/H2O2 system. The competitiveadsorption of H2O2 and downstream catalase activityof H2O2 decomposition were also proposed. Thesubstrate oxidation rate of high-valent iron species reached 9.25x 10(5) mM(-1) min(-1). These results clarified the intrinsic kinetic principle and interfacialreaction mechanism of 2-MeOP oxidative coupling catalyzed by K x FeOCl, offering valuable insights for optimizingreaction performance and scaling up the process. The K+ intercalated modifiedFeOCl material withperoxidase-like catalytic activity enables the oxidative couplingpolymerization of pollutants similar to the humification process andhas significant potential in pollutant treatment.