{"title":"诺氟沙星抗生素在掺硼金刚石阳极上的降解:动力学、途径和机制","authors":"Dandi Zhao , Chongyuan Zhai , Yapeng He , Buming Chen , Chao Gao , Hui Huang , Zhongcheng Guo","doi":"10.1016/j.jtice.2023.104826","DOIUrl":null,"url":null,"abstract":"<div><h3>Background</h3><p>The massive production and irrationally overuse of antibiotics have resulted into the increase and accumulation of antibiotics in the aquatic system. The efficient decomposition of emerging antibiotic pollutants needed to be emphatically discussed considering their persistence and ecological risks.</p></div><div><h3>Method</h3><p>The electrochemical elimination of norfloxacin (NOR) is systematically investigated on BDD anode. The quenching and capturing experiments manifest the predominant radical species. Probable attack locations of reactive radicals are predicted via DFT calculations while evaluating the toxicity evolution of the intermediates during the degradation process by quantitative structure-activity relationship model.</p></div><div><h3>Significant findings</h3><p>The optimal degradation conditions are determined as the initial NOR concentration 50 mg L<sup>−1</sup>, current density 30 mA cm<sup>−2</sup>, 0.05 M Na<sub>2</sub>SO<sub>4</sub> supporting electrolyte, and initial pH 5. The NOR removal rate reach 91.0% with apparent rate constants 0.396 h<sup>−1</sup> after 360 min electrolysis. The <sup>•</sup>OH and SO<sub>4</sub><sup>•−</sup> reactive radicals contribute to the NOR degradation. Possible degradation pathways of NOR mainly include defluorination, decarboxylation, piperazine ring cleavage, and quinolone group transformation, ultimately achieving complete mineralization. The toxicity evolution of the intermediates suggests a low ecotoxicological risk of the anodic oxidation of NOR on BDD anode.</p></div>","PeriodicalId":381,"journal":{"name":"Journal of the Taiwan Institute of Chemical Engineers","volume":null,"pages":null},"PeriodicalIF":5.5000,"publicationDate":"2023-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"1","resultStr":"{\"title\":\"Insights into the degradation of norfloxacin antibiotics on boron-doped diamond anode: Kinetics, pathways and mechanisms\",\"authors\":\"Dandi Zhao , Chongyuan Zhai , Yapeng He , Buming Chen , Chao Gao , Hui Huang , Zhongcheng Guo\",\"doi\":\"10.1016/j.jtice.2023.104826\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><h3>Background</h3><p>The massive production and irrationally overuse of antibiotics have resulted into the increase and accumulation of antibiotics in the aquatic system. The efficient decomposition of emerging antibiotic pollutants needed to be emphatically discussed considering their persistence and ecological risks.</p></div><div><h3>Method</h3><p>The electrochemical elimination of norfloxacin (NOR) is systematically investigated on BDD anode. The quenching and capturing experiments manifest the predominant radical species. Probable attack locations of reactive radicals are predicted via DFT calculations while evaluating the toxicity evolution of the intermediates during the degradation process by quantitative structure-activity relationship model.</p></div><div><h3>Significant findings</h3><p>The optimal degradation conditions are determined as the initial NOR concentration 50 mg L<sup>−1</sup>, current density 30 mA cm<sup>−2</sup>, 0.05 M Na<sub>2</sub>SO<sub>4</sub> supporting electrolyte, and initial pH 5. The NOR removal rate reach 91.0% with apparent rate constants 0.396 h<sup>−1</sup> after 360 min electrolysis. The <sup>•</sup>OH and SO<sub>4</sub><sup>•−</sup> reactive radicals contribute to the NOR degradation. Possible degradation pathways of NOR mainly include defluorination, decarboxylation, piperazine ring cleavage, and quinolone group transformation, ultimately achieving complete mineralization. The toxicity evolution of the intermediates suggests a low ecotoxicological risk of the anodic oxidation of NOR on BDD anode.</p></div>\",\"PeriodicalId\":381,\"journal\":{\"name\":\"Journal of the Taiwan Institute of Chemical Engineers\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.5000,\"publicationDate\":\"2023-04-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"1\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of the Taiwan Institute of Chemical Engineers\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1876107023001554\",\"RegionNum\":3,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the Taiwan Institute of Chemical Engineers","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1876107023001554","RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 1
摘要
抗生素的大量生产和不合理的过度使用导致了水生系统中抗生素的增加和积累。考虑到新出现的抗生素污染物的持久性和生态风险,需要重点讨论其有效分解。方法系统研究了BDD阳极对诺氟沙星(NOR)的电化学去除。猝灭和捕获实验显示了优势自由基种类。通过DFT计算预测活性自由基的可能攻击位置,并通过定量构效关系模型评价中间体在降解过程中的毒性演变。优化的降解条件为初始NOR浓度50 mg L−1,电流密度30 mA cm−2,支撑电解质Na2SO4 0.05 M,初始pH 5。电解360 min后,硝态氮的去除率达到91.0%,表观速率常数0.396 h−1。•OH和SO4•−活性自由基有助于NOR的降解。NOR可能的降解途径主要包括脱氟、脱羧、哌嗪环裂解、喹诺酮基转化等,最终实现完全矿化。中间体的毒性演变表明,在BDD阳极上阳极氧化NOR的生态毒理学风险较低。
Insights into the degradation of norfloxacin antibiotics on boron-doped diamond anode: Kinetics, pathways and mechanisms
Background
The massive production and irrationally overuse of antibiotics have resulted into the increase and accumulation of antibiotics in the aquatic system. The efficient decomposition of emerging antibiotic pollutants needed to be emphatically discussed considering their persistence and ecological risks.
Method
The electrochemical elimination of norfloxacin (NOR) is systematically investigated on BDD anode. The quenching and capturing experiments manifest the predominant radical species. Probable attack locations of reactive radicals are predicted via DFT calculations while evaluating the toxicity evolution of the intermediates during the degradation process by quantitative structure-activity relationship model.
Significant findings
The optimal degradation conditions are determined as the initial NOR concentration 50 mg L−1, current density 30 mA cm−2, 0.05 M Na2SO4 supporting electrolyte, and initial pH 5. The NOR removal rate reach 91.0% with apparent rate constants 0.396 h−1 after 360 min electrolysis. The •OH and SO4•− reactive radicals contribute to the NOR degradation. Possible degradation pathways of NOR mainly include defluorination, decarboxylation, piperazine ring cleavage, and quinolone group transformation, ultimately achieving complete mineralization. The toxicity evolution of the intermediates suggests a low ecotoxicological risk of the anodic oxidation of NOR on BDD anode.
期刊介绍:
Journal of the Taiwan Institute of Chemical Engineers (formerly known as Journal of the Chinese Institute of Chemical Engineers) publishes original works, from fundamental principles to practical applications, in the broad field of chemical engineering with special focus on three aspects: Chemical and Biomolecular Science and Technology, Energy and Environmental Science and Technology, and Materials Science and Technology. Authors should choose for their manuscript an appropriate aspect section and a few related classifications when submitting to the journal online.