文献类型：期刊文献

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

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

机构：[1]East China Univ Sci & Technol, Sch Resources & Environm Engn, State Environm Protect Key Lab Environm Risk Asses, Shanghai 200237, Peoples R China;[2]Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200092, Peoples R China;[3]Tongji Univ, Coll Environm Sci & Engn, State Key Lab Pollut Control & Resource Reuse, Shanghai 200092, Peoples R China;[4]Shanghai Acad Environm Sci, Shanghai 200233, Peoples R China

年份：2024

卷号：37

起止页码：78

外文期刊名：ENGINEERING

收录：;EI(收录号：20242316189779);WOS:【SCI-EXPANDED(收录号:WOS:001284280600001)】；

基金：This study was 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 Munici-pality's Yangfan Special Project (23YF1408400) and the Fundamen-tal Research Funds for the Central Universities.

语种：英文

外文关键词：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 (CO2-)-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 CO2-, with approximately 100% of Cl- and 46% of F- released 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 CO2-. Moreover, CO2--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 CO2--based ARPs in real life. Overall, this study elucidates the feasibility of CO2- for the simultaneous degradation, dehalogenation, and detoxification of halogenated antibiotics and provides a promising method for their regulation during water or wastewater treatment. (c) 2024 THE AUTHORS. Published by Elsevier LTD on behalf of Chinese Academy of Engineering and Higher Education Press Limited Company. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).