Roles of structure defect, oxygen groups and heteroatom doping on carbon in nonradical oxidation of water contaminants
文献类型： 外文期刊
作者： Wang, Jun 1 ; Duan, Xiaoguang 2 ; Gao, Jian 1 ; Shen, Yi 4 ; Feng, Xiaohui 5 ; Yu, Zijun 1 ; Tan, Xiaoyao 1 ; Liu, Shaomi 1 ;
作者机构： 1.Tiangong Univ, Dept Chem Engn, State Key Lab Separat Membranes & Membrane Proc, Tianjin 300387, Peoples R China
2.Univ Adelaide, Sch Chem Engn & Adv Mat, Adelaide, SA 5005, Australia
3.Tiangong Univ, Sch Environm Sci & Engn, Tianjin 300387, Peoples R China
4.Zhejiang Univ Technol, Coll Environm, Hangzhou 310032, Peoples R China
5.Chinese Acad Agr Sci, Inst Anim Sci, State Key Lab Anim Nutr, Beijing, Peoples R China
6.Beijing Univ Chem Technol, Coll Chem Engn, Beijing 100029, Peoples R China
关键词： Ionic liquids; Nonradical degradation; Pharmaceutical contaminants; Carbocatalysis; Peroxymonosulfate
期刊名称：WATER RESEARCH （ 影响因子：11.236； 五年影响因子：11.547 ）
ISSN： 0043-1354
年卷期： 2020 年 185 卷
页码：
收录情况： SCI
摘要： A rational design of structure-tailored and functionalized nanocarbons for peroxymonosulfate (PMS) activation is important in metal-free catalysis for degradation of water contaminants. In this work, we employed ionic liquids (ILs) for synthesis of porous carbon materials (PCMs) as a PMS activator for oxidative removal of naproxen and systematically investigated the functions of structure defects, oxygen functional groups and heteroatom doping toward the catalytic oxidation. A positive linear correlation between reaction rate constants and carbon defect ratios of PCMs revealed that the structural defects played an important role in PMS activation. Electron paramagnetic resonance (EPR) spectra, radical quenching experiments and electrochemical analysis tests verified nonradical-dominated oxidations via electron transfer and O-1(2). Structural vacancies, ketonic C=O groups and graphitic-N atoms on carbons have been revealed to be the active sites for the nonradical pathways via direct electron transfer or generation of O-2(center dot-)/O-1(2). This work provides new insight into the reaction mechanism and structure-performance relationships of the catalytic centers in nonradical oxidation. (C) 2020 Elsevier Ltd. All rights reserved.
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