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

文献类型： 外文期刊

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 ;

作者机构： 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

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

期刊名称：CHEMICAL ENGINEERING JOURNAL （ 影响因子：15.1； 五年影响因子：14.3 ）

ISSN： 1385-8947

年卷期： 2023 年 473 卷

页码：

收录情况： SCI

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.

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