{"title":"通过 C-杂化增加 Mn2O3 的路易斯酸性位点并促进电子传递,从而改善过一硫酸盐活化降解双酚 A 的效果。","authors":"Xinglong Zhang, Qia Zhao, Huan He, Caiyan Zhang, Lele Zhao, Baoning Li","doi":"10.1016/j.envres.2024.120409","DOIUrl":null,"url":null,"abstract":"<p><p>The surface acidity and electron transfer performance of manganese oxide catalysts significantly affected its performance of peroxymonosulfate (PMS) activation. In this work, Mn<sub>2</sub>O<sub>3</sub> catalyst was prepared by the precipitation method. The C-hybridization Mn<sub>2</sub>O<sub>3</sub>-D (Mn<sub>2</sub>O<sub>3</sub>-D) catalyst prepared with disodium oxalate as a precipitant had more Mn<sup>3+</sup> and Lewis acid sites on the surface, promoting the binding of PMS on the catalyst surface, which exhibited the best performance in inducing PMS activation to degrade bisphenol A (BPA). Quenching experiments and in situ electron spin resonance (ESR) results indicated that radicals and singlet oxygen were not the main reactive oxygen species (ROSs) in the advanced oxidation process. The chemical probe experiment of phenylmethylsulfone (PMSO) showed that the ≡Mn-OOSO<sub>3</sub><sup>-</sup> metastable intermediate formed by the binding of PMS with Mn sites on the catalyst surface was important active species for contaminants degradation. Contaminants combined with intermediates on the catalyst surface to form the electron transfer channels, which were directly degraded through oxygen-atom-transfer pathway and single-electron-transfer pathway. And the hybridization of C promoted the electron transfer during this process. This work further elucidated the reaction mechanism of PMS activation by manganese oxides, and proposed new ideas for the design of MnO<sub>x</sub> catalysts for efficient activation of PMS.</p>","PeriodicalId":312,"journal":{"name":"Environmental Research","volume":" ","pages":"120409"},"PeriodicalIF":7.7000,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Increasing Lewis acidic sites and promoting electron transfer of Mn<sub>2</sub>O<sub>3</sub> by C-hybridization to improve the peroxymonosulfate activation for Bisphenol A degradation.\",\"authors\":\"Xinglong Zhang, Qia Zhao, Huan He, Caiyan Zhang, Lele Zhao, Baoning Li\",\"doi\":\"10.1016/j.envres.2024.120409\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>The surface acidity and electron transfer performance of manganese oxide catalysts significantly affected its performance of peroxymonosulfate (PMS) activation. In this work, Mn<sub>2</sub>O<sub>3</sub> catalyst was prepared by the precipitation method. The C-hybridization Mn<sub>2</sub>O<sub>3</sub>-D (Mn<sub>2</sub>O<sub>3</sub>-D) catalyst prepared with disodium oxalate as a precipitant had more Mn<sup>3+</sup> and Lewis acid sites on the surface, promoting the binding of PMS on the catalyst surface, which exhibited the best performance in inducing PMS activation to degrade bisphenol A (BPA). Quenching experiments and in situ electron spin resonance (ESR) results indicated that radicals and singlet oxygen were not the main reactive oxygen species (ROSs) in the advanced oxidation process. The chemical probe experiment of phenylmethylsulfone (PMSO) showed that the ≡Mn-OOSO<sub>3</sub><sup>-</sup> metastable intermediate formed by the binding of PMS with Mn sites on the catalyst surface was important active species for contaminants degradation. Contaminants combined with intermediates on the catalyst surface to form the electron transfer channels, which were directly degraded through oxygen-atom-transfer pathway and single-electron-transfer pathway. And the hybridization of C promoted the electron transfer during this process. This work further elucidated the reaction mechanism of PMS activation by manganese oxides, and proposed new ideas for the design of MnO<sub>x</sub> catalysts for efficient activation of PMS.</p>\",\"PeriodicalId\":312,\"journal\":{\"name\":\"Environmental Research\",\"volume\":\" \",\"pages\":\"120409\"},\"PeriodicalIF\":7.7000,\"publicationDate\":\"2024-11-20\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Environmental Research\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://doi.org/10.1016/j.envres.2024.120409\",\"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}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Environmental Research","FirstCategoryId":"93","ListUrlMain":"https://doi.org/10.1016/j.envres.2024.120409","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}
Increasing Lewis acidic sites and promoting electron transfer of Mn2O3 by C-hybridization to improve the peroxymonosulfate activation for Bisphenol A degradation.
The surface acidity and electron transfer performance of manganese oxide catalysts significantly affected its performance of peroxymonosulfate (PMS) activation. In this work, Mn2O3 catalyst was prepared by the precipitation method. The C-hybridization Mn2O3-D (Mn2O3-D) catalyst prepared with disodium oxalate as a precipitant had more Mn3+ and Lewis acid sites on the surface, promoting the binding of PMS on the catalyst surface, which exhibited the best performance in inducing PMS activation to degrade bisphenol A (BPA). Quenching experiments and in situ electron spin resonance (ESR) results indicated that radicals and singlet oxygen were not the main reactive oxygen species (ROSs) in the advanced oxidation process. The chemical probe experiment of phenylmethylsulfone (PMSO) showed that the ≡Mn-OOSO3- metastable intermediate formed by the binding of PMS with Mn sites on the catalyst surface was important active species for contaminants degradation. Contaminants combined with intermediates on the catalyst surface to form the electron transfer channels, which were directly degraded through oxygen-atom-transfer pathway and single-electron-transfer pathway. And the hybridization of C promoted the electron transfer during this process. This work further elucidated the reaction mechanism of PMS activation by manganese oxides, and proposed new ideas for the design of MnOx catalysts for efficient activation of PMS.
期刊介绍:
The Environmental Research journal presents a broad range of interdisciplinary research, focused on addressing worldwide environmental concerns and featuring innovative findings. Our publication strives to explore relevant anthropogenic issues across various environmental sectors, showcasing practical applications in real-life settings.