文献类型：期刊文献

中文题名：Simultaneous Degradation, Dehalogenation, and Detoxification of Halogenated Antibiotics by Carbon Dioxide Radical Anions

作者：Yanzhou Ding[1];Xia Yu[1,2];Shuguang Lyu[1,2];Huajun Zhen[1,2];Wentao Zhao[3];Cheng Peng[1,2,4];Jiaxi Wang[1];Yiwen Zhu[1];Chengfei Zhu[1];Lei Zhou[1,2];Qian Sui[1,2]

机构：[1]State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process,School of Resources and Environmental Engineering,East China University of Science and Technology,Shanghai 200237,China;[2]Shanghai Institute of Pollution Control and Ecological Security,Shanghai 200092,China;[3]State Key Laboratory of Pollution Control and Resource Reuse,College of Environmental Science and Engineering,Tongji University,Shanghai 200092,China;[4]Shanghai Academy of Environmental Sciences,Shanghai 200233,China

年份：2024

卷号：37

期号：6

起止页码：78

中文期刊名：Engineering

外文期刊名：工程（英文）

收录：CSTPCD;;Scopus;CSCD:【CSCD2023_2024】；PubMed;

基金：financially supported by the National Natural Science Foundation of China(22176059,21777042,and 22076045);the authors would also like to acknowledge support from the Science and Technology Commission of Shanghai Municipality’s Yangfan Special Project(23YF1408400);the Fundamental Research Funds for the Central Universities.

语种：英文

中文关键词：Carbon dioxide radical anions;Advanced reduction processes;Halogenated antibiotics;Dehalogenation;Detoxification

摘要：Despite the extensive application of advanced oxidation processes(AOPs)in water treatment,the efficiency of AOPs in eliminating various emerging contaminants such as halogenated antibiotics is constrained by a number of factors.Halogen moieties exhibit strong resistance to oxidative radicals,affecting the dehalogenation and detoxification efficiencies.To address these limitations of AOPs,advanced reduction processes(ARPs)have been proposed.Herein,a novel nucleophilic reductant—namely,the carbon dioxide radical anion(CO_(2)^(·-))—is introduced for the simultaneous degradation,dehalogenation,and detoxification of florfenicol(FF),a typical halogenated antibiotic.The results demonstrate that FF is completely eliminated by CO_(2)^(·-),with approximately 100%of Cland 46%of Freleased after 120 min of treatment.Simultaneous detoxification is observed,which exhibits a linear response to the release of free inorganic halogen ions(R^(2)=0.97,p<0.01).The formation of halogen-free products is the primary reason for the superior detoxification performance of this method,in comparison with conventional hydroxyl-radical-based AOPs.Products identification and density functional theory(DFT)calculations reveal the underlying dehalogenation mechanism,in which the chlorine moiety of FF is more susceptible than other moieties to nucleophilic attack by CO_(2)^(·-).Moreover,CO_(2)^(·-)-based ARPs exhibit superior dehalogenation efficiencies(>75%)in degrading a series of halogenated antibiotics,including chloramphenicol(CAP),thiamphenicol(THA),diclofenac(DLF),triclosan(TCS),and ciprofloxacin(CIP).The system shows high tolerance to the pH of the solution and the presence of natural water constituents,and demonstrates an excellent degradation performance in actual groundwater,indicating the strong application potential of CO_(2)^(·-)-based ARPs in real life.Overall,this study elucidates the feasibility of CO_(2)^(·-)for the simultaneous degradation,dehalogenation,and detoxification of halogenated antibiotics and provides a promising method for their regulation during water or wastewater treatment.