{"title":"揭示支撑电解质的内在电化学机理以及纳米二氧化铅电化学氧化四环素的相互作用机理","authors":"Yaxuan Wang, Peitong Cen, Hongyu Wang, Chenxi Li, Ziyin Xia, Guoqing Wu, Meng Li, Lei Huang, Jia Yan, Shaoqi Zhou, Ce-Hui Mo, Hongguo Zhang","doi":"10.1039/d4en00842a","DOIUrl":null,"url":null,"abstract":"Electrochemical oxidation (EO) for the removal of antibiotics is a promising technique because of green and sustainable electrical−to−chemical energy conversion. However, the interaction mechanism between different electrolytes molecule and organic pollution along with the generation pathway of reactive oxygen species remain unclear. Here, the β−PbO2 electrode was successfully prepared and employed as an effective tool for organic pollution removal. The EO process with β−PbO2 electrode and Na2SO4 electrolyte could completely remove tetracycline (TC) and achieve an impressive kinetic rate constant of 0.239 min−1. Quantum chemical calculations confirmed that hydrogen bonding was the primary binding force between TC and Na2SO4. Density functional theory calculations emphasized the key roles of radical and non−radical pathways in TC removal via the key reaction site (O atom in PbO2). Consequently, this study provided a novel insight into the intrinsic electrochemical behavior changes under various electrolyte, paving the way for novel electrochemical process in water treatment applications.","PeriodicalId":73,"journal":{"name":"Environmental Science: Nano","volume":"41 1","pages":""},"PeriodicalIF":5.8000,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Unveiling intrinsic electrochemical mechanism of supporting electrolyte and interaction mechanism in electrochemical oxidation tetracycline with nano-PbO2\",\"authors\":\"Yaxuan Wang, Peitong Cen, Hongyu Wang, Chenxi Li, Ziyin Xia, Guoqing Wu, Meng Li, Lei Huang, Jia Yan, Shaoqi Zhou, Ce-Hui Mo, Hongguo Zhang\",\"doi\":\"10.1039/d4en00842a\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Electrochemical oxidation (EO) for the removal of antibiotics is a promising technique because of green and sustainable electrical−to−chemical energy conversion. However, the interaction mechanism between different electrolytes molecule and organic pollution along with the generation pathway of reactive oxygen species remain unclear. Here, the β−PbO2 electrode was successfully prepared and employed as an effective tool for organic pollution removal. The EO process with β−PbO2 electrode and Na2SO4 electrolyte could completely remove tetracycline (TC) and achieve an impressive kinetic rate constant of 0.239 min−1. Quantum chemical calculations confirmed that hydrogen bonding was the primary binding force between TC and Na2SO4. Density functional theory calculations emphasized the key roles of radical and non−radical pathways in TC removal via the key reaction site (O atom in PbO2). Consequently, this study provided a novel insight into the intrinsic electrochemical behavior changes under various electrolyte, paving the way for novel electrochemical process in water treatment applications.\",\"PeriodicalId\":73,\"journal\":{\"name\":\"Environmental Science: Nano\",\"volume\":\"41 1\",\"pages\":\"\"},\"PeriodicalIF\":5.8000,\"publicationDate\":\"2024-11-12\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Environmental Science: Nano\",\"FirstCategoryId\":\"6\",\"ListUrlMain\":\"https://doi.org/10.1039/d4en00842a\",\"RegionNum\":2,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Environmental Science: Nano","FirstCategoryId":"6","ListUrlMain":"https://doi.org/10.1039/d4en00842a","RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
电化学氧化法(EO)可将电能转化为化学能,是一种绿色、可持续的去除抗生素的技术。然而,不同电解质分子与有机污染之间的相互作用机制以及活性氧的生成途径仍不清楚。在此,我们成功制备了β-PbO2电极,并将其用作去除有机污染的有效工具。使用β-PbO2电极和Na2SO4电解液的环氧乙烷过程可以完全去除四环素(TC),并达到了令人印象深刻的0.239 min-1动力学速率常数。量子化学计算证实,氢键是四环素与 Na2SO4 之间的主要结合力。密度泛函理论计算强调了通过关键反应位点(PbO2 中的 O 原子)去除 TC 的自由基和非自由基途径的关键作用。因此,这项研究为了解不同电解质下的内在电化学行为变化提供了新的视角,为新型电化学工艺在水处理中的应用铺平了道路。
Unveiling intrinsic electrochemical mechanism of supporting electrolyte and interaction mechanism in electrochemical oxidation tetracycline with nano-PbO2
Electrochemical oxidation (EO) for the removal of antibiotics is a promising technique because of green and sustainable electrical−to−chemical energy conversion. However, the interaction mechanism between different electrolytes molecule and organic pollution along with the generation pathway of reactive oxygen species remain unclear. Here, the β−PbO2 electrode was successfully prepared and employed as an effective tool for organic pollution removal. The EO process with β−PbO2 electrode and Na2SO4 electrolyte could completely remove tetracycline (TC) and achieve an impressive kinetic rate constant of 0.239 min−1. Quantum chemical calculations confirmed that hydrogen bonding was the primary binding force between TC and Na2SO4. Density functional theory calculations emphasized the key roles of radical and non−radical pathways in TC removal via the key reaction site (O atom in PbO2). Consequently, this study provided a novel insight into the intrinsic electrochemical behavior changes under various electrolyte, paving the way for novel electrochemical process in water treatment applications.
期刊介绍:
Environmental Science: Nano serves as a comprehensive and high-impact peer-reviewed source of information on the design and demonstration of engineered nanomaterials for environment-based applications. It also covers the interactions between engineered, natural, and incidental nanomaterials with biological and environmental systems. This scope includes, but is not limited to, the following topic areas:
Novel nanomaterial-based applications for water, air, soil, food, and energy sustainability
Nanomaterial interactions with biological systems and nanotoxicology
Environmental fate, reactivity, and transformations of nanoscale materials
Nanoscale processes in the environment
Sustainable nanotechnology including rational nanomaterial design, life cycle assessment, risk/benefit analysis