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{"title":"过渡金属硒化物上的双金属氧化还原驱动 PMS 快速活化以降解磺胺甲噁唑:机理、降解途径和中间体毒性","authors":"Yongming Wang, Qiang Chen, Yuezong Su, Yuxuan He, Jin Qian, Kailin Xu","doi":"10.1002/jctb.7748","DOIUrl":null,"url":null,"abstract":"BACKGROUNDThe increasing presence of antibiotics in aquatic environments poses significant ecological risks, with sulfamethoxazole (SMX) being a prominent example due to its persistence and widespread use in medical and veterinary practices. Advanced oxidation processes, particularly those based on peroxymonosulfate (PMS), have shown promise in degrading such contaminants. This work explored the efficacy of a bimetallic selenide catalyst, FeSe<jats:sub>2</jats:sub>/MoSe<jats:sub>2</jats:sub> (FM), synthesized via a hydrothermal method, for the rapid activation of PMS and subsequent degradation of SMX.RESULTSOver 95% SMX degradation was achieved with a 0.25 g/L catalyst dosage and 1.5 g/L PMS dosage, demonstrating that FM was an effective PMS activator capable of efficiently oxidizing SMX. The EPR tests and quenching experiments confirmed the presence of <jats:sup>1</jats:sup>O<jats:sub>2</jats:sub>, SO<jats:sub>4</jats:sub><jats:sup>•–</jats:sup> and <jats:sup>•</jats:sup>OH in the degradation system, with SO<jats:sub>4</jats:sub><jats:sup>•‐</jats:sup> predominating. The redox cycling of Mo with Fe was involved in the activation of PMS. Moreover, the DFT calculations of the SMX molecule revealed that the vulnerable sites were mainly in the vicinity of the sulfonamide group and the oxygen‐containing group. The toxicity assessment disclosed that most of the primary degradation intermediates of SMX were toxic, while the further small molecule products were non‐toxic.CONCLUSIONThis work underscores the potential of the FM/PMS system as an efficient and sustainable solution for degrading antibiotic contaminants like SMX in water. The low toxicity of the final degradation products further supports the environmental safety of this approach, making it a promising candidate for real‐world water treatment applications. © 2024 Society of Chemical Industry (SCI).","PeriodicalId":15335,"journal":{"name":"Journal of chemical technology and biotechnology","volume":null,"pages":null},"PeriodicalIF":2.8000,"publicationDate":"2024-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Rapid activation of PMS driven by bimetallic redox on transition metal selenides for sulfamethoxazole degradation: mechanism, degradation pathway and intermediates toxicity\",\"authors\":\"Yongming Wang, Qiang Chen, Yuezong Su, Yuxuan He, Jin Qian, Kailin Xu\",\"doi\":\"10.1002/jctb.7748\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"BACKGROUNDThe increasing presence of antibiotics in aquatic environments poses significant ecological risks, with sulfamethoxazole (SMX) being a prominent example due to its persistence and widespread use in medical and veterinary practices. Advanced oxidation processes, particularly those based on peroxymonosulfate (PMS), have shown promise in degrading such contaminants. This work explored the efficacy of a bimetallic selenide catalyst, FeSe<jats:sub>2</jats:sub>/MoSe<jats:sub>2</jats:sub> (FM), synthesized via a hydrothermal method, for the rapid activation of PMS and subsequent degradation of SMX.RESULTSOver 95% SMX degradation was achieved with a 0.25 g/L catalyst dosage and 1.5 g/L PMS dosage, demonstrating that FM was an effective PMS activator capable of efficiently oxidizing SMX. The EPR tests and quenching experiments confirmed the presence of <jats:sup>1</jats:sup>O<jats:sub>2</jats:sub>, SO<jats:sub>4</jats:sub><jats:sup>•–</jats:sup> and <jats:sup>•</jats:sup>OH in the degradation system, with SO<jats:sub>4</jats:sub><jats:sup>•‐</jats:sup> predominating. The redox cycling of Mo with Fe was involved in the activation of PMS. Moreover, the DFT calculations of the SMX molecule revealed that the vulnerable sites were mainly in the vicinity of the sulfonamide group and the oxygen‐containing group. The toxicity assessment disclosed that most of the primary degradation intermediates of SMX were toxic, while the further small molecule products were non‐toxic.CONCLUSIONThis work underscores the potential of the FM/PMS system as an efficient and sustainable solution for degrading antibiotic contaminants like SMX in water. The low toxicity of the final degradation products further supports the environmental safety of this approach, making it a promising candidate for real‐world water treatment applications. © 2024 Society of Chemical Industry (SCI).\",\"PeriodicalId\":15335,\"journal\":{\"name\":\"Journal of chemical technology and biotechnology\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":2.8000,\"publicationDate\":\"2024-09-06\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of chemical technology and biotechnology\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1002/jctb.7748\",\"RegionNum\":4,\"RegionCategory\":\"生物学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"BIOTECHNOLOGY & APPLIED MICROBIOLOGY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of chemical technology and biotechnology","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1002/jctb.7748","RegionNum":4,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"BIOTECHNOLOGY & APPLIED MICROBIOLOGY","Score":null,"Total":0}
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Rapid activation of PMS driven by bimetallic redox on transition metal selenides for sulfamethoxazole degradation: mechanism, degradation pathway and intermediates toxicity
BACKGROUNDThe increasing presence of antibiotics in aquatic environments poses significant ecological risks, with sulfamethoxazole (SMX) being a prominent example due to its persistence and widespread use in medical and veterinary practices. Advanced oxidation processes, particularly those based on peroxymonosulfate (PMS), have shown promise in degrading such contaminants. This work explored the efficacy of a bimetallic selenide catalyst, FeSe2 /MoSe2 (FM), synthesized via a hydrothermal method, for the rapid activation of PMS and subsequent degradation of SMX.RESULTSOver 95% SMX degradation was achieved with a 0.25 g/L catalyst dosage and 1.5 g/L PMS dosage, demonstrating that FM was an effective PMS activator capable of efficiently oxidizing SMX. The EPR tests and quenching experiments confirmed the presence of 1 O2 , SO4 •– and • OH in the degradation system, with SO4 •‐ predominating. The redox cycling of Mo with Fe was involved in the activation of PMS. Moreover, the DFT calculations of the SMX molecule revealed that the vulnerable sites were mainly in the vicinity of the sulfonamide group and the oxygen‐containing group. The toxicity assessment disclosed that most of the primary degradation intermediates of SMX were toxic, while the further small molecule products were non‐toxic.CONCLUSIONThis work underscores the potential of the FM/PMS system as an efficient and sustainable solution for degrading antibiotic contaminants like SMX in water. The low toxicity of the final degradation products further supports the environmental safety of this approach, making it a promising candidate for real‐world water treatment applications. © 2024 Society of Chemical Industry (SCI).