Pengcheng Yao , Wei Wang , Hui Wu , Ziming Wang , Yawei Xie , Jinjuan Zhang , Qiannan Jin , Aiju You
{"title":"Activation of peroxydisulfate by iron dichloride with hydroxylamine promoted sulfapyridine degradation","authors":"Pengcheng Yao , Wei Wang , Hui Wu , Ziming Wang , Yawei Xie , Jinjuan Zhang , Qiannan Jin , Aiju You","doi":"10.1016/j.emcon.2024.100350","DOIUrl":null,"url":null,"abstract":"<div><p>Sulfapyridine (SPY) is a ubiquitous environmental contaminant belonging to the sulfonamide antibiotics. Previous studies showed that hydroxylamine (HA) can improve the performance of advanced oxidation processes (AOPs) by promoting Fe(II) regeneration, yet the reaction mechanisms were not elucidated. Therefore, the role of HA and the degradation mechanisms of SPY were systematically studied therein. The SPY degradation efficiency increased from 77.5 % to 91.6 % after HA was added. With radical scavenger experiment, a function of HA to promote <sup>•</sup>OH production for SPY degradation was clarified. The major radical from SO<sub>4</sub><sup>•-</sup> and <sup>•</sup>OH to <sup>•</sup>OH with addition of HA in Fe(II)/potassium peroxydisulfate (PDS). Results showed that alkali, acid condition and high PDS concentration all contributed to SPY degradation. According to experimental results, density functional theory (DFT) was used to calculate the degradation pathway of SPY. Rate-limiting path was obtained by comparing the rate constants calculated from the transition-state theory. The cleavage of C–C bond in benzene ring with the slowest rate was essential to degrade SPY, which not only promotes the mineralization of SPY, but also prevent the production of toxic TPs effectively. This study provides valuable insight into the SPY degradation in HA/Fe(II)/PDS.</p></div>","PeriodicalId":11539,"journal":{"name":"Emerging Contaminants","volume":null,"pages":null},"PeriodicalIF":5.3000,"publicationDate":"2024-04-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2405665024000519/pdfft?md5=30f8cc3ea8b3763fb8544cfc93b40fc1&pid=1-s2.0-S2405665024000519-main.pdf","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Emerging Contaminants","FirstCategoryId":"1087","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2405665024000519","RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENVIRONMENTAL SCIENCES","Score":null,"Total":0}
引用次数: 0
Abstract
Sulfapyridine (SPY) is a ubiquitous environmental contaminant belonging to the sulfonamide antibiotics. Previous studies showed that hydroxylamine (HA) can improve the performance of advanced oxidation processes (AOPs) by promoting Fe(II) regeneration, yet the reaction mechanisms were not elucidated. Therefore, the role of HA and the degradation mechanisms of SPY were systematically studied therein. The SPY degradation efficiency increased from 77.5 % to 91.6 % after HA was added. With radical scavenger experiment, a function of HA to promote •OH production for SPY degradation was clarified. The major radical from SO4•- and •OH to •OH with addition of HA in Fe(II)/potassium peroxydisulfate (PDS). Results showed that alkali, acid condition and high PDS concentration all contributed to SPY degradation. According to experimental results, density functional theory (DFT) was used to calculate the degradation pathway of SPY. Rate-limiting path was obtained by comparing the rate constants calculated from the transition-state theory. The cleavage of C–C bond in benzene ring with the slowest rate was essential to degrade SPY, which not only promotes the mineralization of SPY, but also prevent the production of toxic TPs effectively. This study provides valuable insight into the SPY degradation in HA/Fe(II)/PDS.
期刊介绍:
Emerging Contaminants is an outlet for world-leading research addressing problems associated with environmental contamination caused by emerging contaminants and their solutions. Emerging contaminants are defined as chemicals that are not currently (or have been only recently) regulated and about which there exist concerns regarding their impact on human or ecological health. Examples of emerging contaminants include disinfection by-products, pharmaceutical and personal care products, persistent organic chemicals, and mercury etc. as well as their degradation products. We encourage papers addressing science that facilitates greater understanding of the nature, extent, and impacts of the presence of emerging contaminants in the environment; technology that exploits original principles to reduce and control their environmental presence; as well as the development, implementation and efficacy of national and international policies to protect human health and the environment from emerging contaminants.