文献类型：期刊文献

英文题名：Synthesis of a trivalent copper complex for efficient degradation of antibiotic ofloxacin

作者：Hong, Hui[1];Xu, Minghao[1];Yang, Xuerui[1,2];Zhou, Lei[1,2,3];Chovelon, Jean-Marc[4];Xiu, Guangli[1,2,3]

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]East China Univ Sci & Technol, Sch Resources & Environm Engn, Shanghai Environm Protect Key Lab Environm Stand &, Shanghai 200237, Peoples R China;[3]Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200092, Peoples R China;[4]Univ Lyon, Univ Claude Bernard Lyon 1, CNRS, IRCELYON, 2 Ave Albert Einstein, F-69626 Villeurbanne, France

年份：2024

卷号：479

外文期刊名：CHEMICAL ENGINEERING JOURNAL

收录：;EI(收录号：20240315406594);WOS:【SCI-EXPANDED(收录号:WOS:001156117400001)】；

基金：The current study received financial support from the National Natural Science Foundation of China (No. 22306064 & 22176059) , the Natural Science Foundation of Shanghai (23ZR1417500) , Fellowship of China Postdoctoral Science Foundation (2023M731085) , and the Fundamental Research Funds for the Central Universities. We also extend our gratitude to Dr. Ting Wu for providing invaluable technical assistance in identification of products by using HR -MS.

语种：英文

外文关键词：Cu(III) species; Ofloxacin; Advanced oxidation processes; Reaction mechanism; Density functional theory calculations

摘要：Copper-based catalysts have been widely used in heterogeneous advanced oxidation processes (AOPs) to degrade emerging contaminants, with trivalent copper species (Cu(III)) often identified as crucial intermediates. However, the current understanding of the reactivity and potential oxidation mechanism associated with such reactive species remains quite limited. In the present study, a stable Cu(III) complex was synthesized, and its reactivity towards a typical fluoroquinolone antibiotic, ofloxacin (OFX), was comprehensively investigated. The results revealed that Cu(III) itself functioned as the primary oxidizing agent instead of secondary hydroxyl radicals generated during OFX decomposition, which exhibited high reactivity over a wide pH range (3.0-9.0) with molar ratio of Cu(III) to OFX between 1:2 and 3:1. Interestingly, prevalent constituents of natural water, including (bi)carbonate (0-10 mM), chloride (0-10 mM), nitrate (0-10 mM) and humic acid (0-30 mg/L), displayed minimal influence on the oxidation efficiency of Cu(III). Piperazine moiety was identified as the primary reaction site, and three different pathways including tertiary amine oxidation, hydroxylation, and Ndemethylation process were proposed. The detailed oxidation mechanisms were further illustrated by density functional theory (DFT) calculations. This study contributes to the theoretical foundation for investigating the mechanism of Cu(III)-mediated oxidation of antibiotics.