文献类型：期刊文献

英文题名：Modulating the redox couples of graphene-like NBC-TiO2@FeMn through forming photo-Fenton system for boosting persulfate activation to accelerate the contaminant degradation

作者：Bai, He[1];Yang, Yuxiang[1];Zhang, Jining[2];Yang, Yubing[3];Yuan, Hongming[4];Dong, Mengyang[1];Wang, Chengyin[5];Ni, Chaoying[6]

机构：[1]East China Univ Sci & Technol, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[2]Shanghai Acad Agr Sci, Ecoenvironm Protect Res Inst, Shanghai 201403, Peoples R China;[3]Liuzhou Inst Technol, Liuzhou 545616, Guangxi, Peoples R China;[4]Jilin Univ, State Key Lab Inorgan Synth & Preparat Chem, Changchun 130012, Peoples R China;[5]Yangzhou Univ, Coll Chem & Chem Engn, Yangzhou 225002, Peoples R China;[6]Univ Delaware, Dept Mat Sci & Engn, Newark, DE 19716 USA

年份：2023

卷号：473

外文期刊名：CHEMICAL ENGINEERING JOURNAL

收录：;EI(收录号：20233414587834);WOS:【SCI-EXPANDED(收录号:WOS:001092591700001)】；

基金：This work was supported by the National Natural Science Foundation of China (20577010, 20971043), and the Open Project Program of State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Jilin University.

语种：英文

外文关键词：Graphene-like biochar; Photo-Fenton; Redox cycles; FeMn LDH; SR-AOPs

摘要：The sluggish cycling of redox couples hampers the practical application of catalysts in contaminant degradation. Herein, a novel strategy was introduced by constructing a photo-Fenton system onto the graphene-like NBC to realize the ultrafast modulating of redox couples during the contaminant degradation. The constructed NBCTiO2@FeMn (NBTF) exhibits a higher proportion of reductive redox couples (Fe (II)/Mn (II)) after the degradation, which is attributable to the photo-Fenton system and the graphene-like NBC with high electron transfer efficiency. Density functional theory (DFT) calculations also confirm that constructing the photo-Fenton system on graphene-like NBC greatly enhances electron transfer, enabling the modulation of redox couples during the degradation process. During activation, various reactive oxygen species (including center dot OH, SO4 center dot-, high-valent metal oxides, and non-radical pathways) are generated, effectively degrading pulp wastewater Tetrachloroguaiacol (TeCG) with a degradation efficiency of 98.8 % within 14 min. Quenching experiments and EPR spectroscopic analysis indicate that the degradation of TeCG is mainly mediated by hydroxyl radicals (center dot OH) and sulfate radicals (SO4 center dot-) as predominant pathways, while high-valent metal oxides, O-1(2) and direct electron transfer mechanisms act in a cooperative manner. Substitution reaction on active sites reveal that both FeMn LDH and graphene-like NBC are identified as the main active sites, with Mn exhibiting superior PMS activation compared to Fe. A possible degradation pathway of TeCG is proposed, and a decrease in the toxicity of intermediates is observed. This study provides a new perspective on the modulation of redox couples in SR-AOPs to realize sustainable pollutants degradation.