Chang Cai , Tian Jiang , Honggen Peng , Xiaoxiao Fu , Chunyang Nie , Zhimin Ao
{"title":"1T/2H-MoS2阴极对过氧单硫酸盐的持续活化增强了有机污染物的去除:基于表面mo -过氧单硫酸盐配合物的性能和非自由基活化机制","authors":"Chang Cai , Tian Jiang , Honggen Peng , Xiaoxiao Fu , Chunyang Nie , Zhimin Ao","doi":"10.1016/j.cej.2025.164474","DOIUrl":null,"url":null,"abstract":"<div><div>MoS<sub>2</sub> is an effective catalyst for peroxymonosulfate (PMS) activation, but its poor reusability hinders the practical application. To address this issue, we immobilized multiphasic 1T/2H-MoS<sub>2</sub> onto a carbon fiber cloth (1T/2H-MoS<sub>2</sub>@CFC) and utilized it as the cathode to sustainably activate PMS because electrons supplied by cathode can regenerate Mo catalytic sites. In addition, the electrochemical 1T/2H-MoS<sub>2</sub>@CFC cathode/PMS system manifests enhanced removal performance of aqueous organic pollutants by coupling PMS activation with electrosorption of organics. Through integrated experimental and theoretical investigations, we found that negative polarization of 1T/2H-MoS<sub>2</sub> makes the electrostatic potential of Mo active sites in 1T/2H-MoS<sub>2</sub> more positive and l<sub>S-O</sub> of adsorbed HSO<sub>5</sub><sup>−</sup> longer, while positive polarization does the opposite. Accordingly, 1T/2H-MoS<sub>2</sub> cathode attains higher PMS activation efficiency than the anode and induces formation of nonradical surface Mo-PMS complexes, differing from the activation pathway induced by 1T/2H-MoS<sub>2</sub> anode which involves •OH, SO<sub>4</sub><sup>•-</sup> and <sup>1</sup>O<sub>2</sub>. Finally, the degradation performance of 1T/2H-MoS<sub>2</sub>@CFC cathode/PMS system in different real water matrices was assessed and it was found to perform effectively in all cases. Our findings offer an efficient and economical electrochemical oxidative system for water decontamination.</div></div>","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"518 ","pages":"Article 164474"},"PeriodicalIF":13.2000,"publicationDate":"2025-06-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Sustainable peroxymonosulfate activation by 1T/2H-MoS2 cathode for enhanced removal of organic pollutants: Performance and nonradical activation mechanism based on surface Mo-peroxymonosulfate complexes\",\"authors\":\"Chang Cai , Tian Jiang , Honggen Peng , Xiaoxiao Fu , Chunyang Nie , Zhimin Ao\",\"doi\":\"10.1016/j.cej.2025.164474\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>MoS<sub>2</sub> is an effective catalyst for peroxymonosulfate (PMS) activation, but its poor reusability hinders the practical application. To address this issue, we immobilized multiphasic 1T/2H-MoS<sub>2</sub> onto a carbon fiber cloth (1T/2H-MoS<sub>2</sub>@CFC) and utilized it as the cathode to sustainably activate PMS because electrons supplied by cathode can regenerate Mo catalytic sites. In addition, the electrochemical 1T/2H-MoS<sub>2</sub>@CFC cathode/PMS system manifests enhanced removal performance of aqueous organic pollutants by coupling PMS activation with electrosorption of organics. Through integrated experimental and theoretical investigations, we found that negative polarization of 1T/2H-MoS<sub>2</sub> makes the electrostatic potential of Mo active sites in 1T/2H-MoS<sub>2</sub> more positive and l<sub>S-O</sub> of adsorbed HSO<sub>5</sub><sup>−</sup> longer, while positive polarization does the opposite. Accordingly, 1T/2H-MoS<sub>2</sub> cathode attains higher PMS activation efficiency than the anode and induces formation of nonradical surface Mo-PMS complexes, differing from the activation pathway induced by 1T/2H-MoS<sub>2</sub> anode which involves •OH, SO<sub>4</sub><sup>•-</sup> and <sup>1</sup>O<sub>2</sub>. Finally, the degradation performance of 1T/2H-MoS<sub>2</sub>@CFC cathode/PMS system in different real water matrices was assessed and it was found to perform effectively in all cases. Our findings offer an efficient and economical electrochemical oxidative system for water decontamination.</div></div>\",\"PeriodicalId\":270,\"journal\":{\"name\":\"Chemical Engineering Journal\",\"volume\":\"518 \",\"pages\":\"Article 164474\"},\"PeriodicalIF\":13.2000,\"publicationDate\":\"2025-06-07\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemical Engineering Journal\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1385894725053100\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Engineering Journal","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1385894725053100","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Sustainable peroxymonosulfate activation by 1T/2H-MoS2 cathode for enhanced removal of organic pollutants: Performance and nonradical activation mechanism based on surface Mo-peroxymonosulfate complexes
MoS2 is an effective catalyst for peroxymonosulfate (PMS) activation, but its poor reusability hinders the practical application. To address this issue, we immobilized multiphasic 1T/2H-MoS2 onto a carbon fiber cloth (1T/2H-MoS2@CFC) and utilized it as the cathode to sustainably activate PMS because electrons supplied by cathode can regenerate Mo catalytic sites. In addition, the electrochemical 1T/2H-MoS2@CFC cathode/PMS system manifests enhanced removal performance of aqueous organic pollutants by coupling PMS activation with electrosorption of organics. Through integrated experimental and theoretical investigations, we found that negative polarization of 1T/2H-MoS2 makes the electrostatic potential of Mo active sites in 1T/2H-MoS2 more positive and lS-O of adsorbed HSO5− longer, while positive polarization does the opposite. Accordingly, 1T/2H-MoS2 cathode attains higher PMS activation efficiency than the anode and induces formation of nonradical surface Mo-PMS complexes, differing from the activation pathway induced by 1T/2H-MoS2 anode which involves •OH, SO4•- and 1O2. Finally, the degradation performance of 1T/2H-MoS2@CFC cathode/PMS system in different real water matrices was assessed and it was found to perform effectively in all cases. Our findings offer an efficient and economical electrochemical oxidative system for water decontamination.
期刊介绍:
The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.