{"title":"热辅助可见光催化 PMS 降解双氯芬酸:掺锰 g-C3N4 催化剂和协同催化机理","authors":"Qinglu Yuan, Peize Wang, Mengjie Fan, Yuan Xu, Yingwen Chen","doi":"10.1007/s10562-024-04817-5","DOIUrl":null,"url":null,"abstract":"<div><p>Different manganese salt precursor-doped g-C<sub>3</sub>N<sub>4</sub> catalysts prepared by the mixed calcination method were applied in the heat-assisted visible light catalytic peroxymonosulfate (PMS) activation (Heat/Vis/PMS) system for the degradation of diclofenac (DCF). Under this Heat/Vis/PMS system, the CN-Mn-S catalyst using MnSO<sub>4</sub> as the manganese salt precursor showed the optimal DCF degradation efficiency (96.9%) with the fastest reaction rate (0.1607 min<sup>−1</sup>). Besides, with the advantages of large specific surface area, high Mn<sub>3</sub>O<sub>4</sub> generation, and good visible light absorption performance, CN-Mn-S catalyst also maintained excellent catalytic activity after five cycles. Electron paramagnetic resonance (EPR) analysis revealed that the generation of active species with relatively high contribution to DCF degradation, including generation of superoxide anion (O<sub>2</sub>·<sup>−</sup>) and singlet oxygen (<sup>1</sup>O<sub>2</sub>), were significantly increased in the CN-Mn-S/Heat/Vis/PMS system. Meanwhile, combined with the analysis of influence factor experiments and the DCF degradation characteristics, the CN-Mn-S/Heat/Vis/PMS system was able to maintain excellent DCF degradation ability in complex environments. This work provides a new idea for the application of PMS in real environment.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"154 12","pages":"6254 - 6270"},"PeriodicalIF":2.3000,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Heat-Assisted Visible Light Catalytic PMS for Diclofenac Degradation: Mn-Doped g-C3N4 Catalysts and Synergistic Catalytic Mechanism\",\"authors\":\"Qinglu Yuan, Peize Wang, Mengjie Fan, Yuan Xu, Yingwen Chen\",\"doi\":\"10.1007/s10562-024-04817-5\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Different manganese salt precursor-doped g-C<sub>3</sub>N<sub>4</sub> catalysts prepared by the mixed calcination method were applied in the heat-assisted visible light catalytic peroxymonosulfate (PMS) activation (Heat/Vis/PMS) system for the degradation of diclofenac (DCF). Under this Heat/Vis/PMS system, the CN-Mn-S catalyst using MnSO<sub>4</sub> as the manganese salt precursor showed the optimal DCF degradation efficiency (96.9%) with the fastest reaction rate (0.1607 min<sup>−1</sup>). Besides, with the advantages of large specific surface area, high Mn<sub>3</sub>O<sub>4</sub> generation, and good visible light absorption performance, CN-Mn-S catalyst also maintained excellent catalytic activity after five cycles. Electron paramagnetic resonance (EPR) analysis revealed that the generation of active species with relatively high contribution to DCF degradation, including generation of superoxide anion (O<sub>2</sub>·<sup>−</sup>) and singlet oxygen (<sup>1</sup>O<sub>2</sub>), were significantly increased in the CN-Mn-S/Heat/Vis/PMS system. Meanwhile, combined with the analysis of influence factor experiments and the DCF degradation characteristics, the CN-Mn-S/Heat/Vis/PMS system was able to maintain excellent DCF degradation ability in complex environments. This work provides a new idea for the application of PMS in real environment.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>\",\"PeriodicalId\":508,\"journal\":{\"name\":\"Catalysis Letters\",\"volume\":\"154 12\",\"pages\":\"6254 - 6270\"},\"PeriodicalIF\":2.3000,\"publicationDate\":\"2024-09-13\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Catalysis Letters\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s10562-024-04817-5\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Catalysis Letters","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s10562-024-04817-5","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Heat-Assisted Visible Light Catalytic PMS for Diclofenac Degradation: Mn-Doped g-C3N4 Catalysts and Synergistic Catalytic Mechanism
Different manganese salt precursor-doped g-C3N4 catalysts prepared by the mixed calcination method were applied in the heat-assisted visible light catalytic peroxymonosulfate (PMS) activation (Heat/Vis/PMS) system for the degradation of diclofenac (DCF). Under this Heat/Vis/PMS system, the CN-Mn-S catalyst using MnSO4 as the manganese salt precursor showed the optimal DCF degradation efficiency (96.9%) with the fastest reaction rate (0.1607 min−1). Besides, with the advantages of large specific surface area, high Mn3O4 generation, and good visible light absorption performance, CN-Mn-S catalyst also maintained excellent catalytic activity after five cycles. Electron paramagnetic resonance (EPR) analysis revealed that the generation of active species with relatively high contribution to DCF degradation, including generation of superoxide anion (O2·−) and singlet oxygen (1O2), were significantly increased in the CN-Mn-S/Heat/Vis/PMS system. Meanwhile, combined with the analysis of influence factor experiments and the DCF degradation characteristics, the CN-Mn-S/Heat/Vis/PMS system was able to maintain excellent DCF degradation ability in complex environments. This work provides a new idea for the application of PMS in real environment.
期刊介绍:
Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis.
The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.