{"title":"高金属负载亚纳米簇催化剂通过生成高价铜增强了新污染物降解的 Fenton 类反应活性","authors":"","doi":"10.1016/j.seppur.2024.129794","DOIUrl":null,"url":null,"abstract":"<div><div>High-valent copper (Cu(III)) species are crucial intermediates in C<img>H bond functionalization within both the biological and biomimetic processes, facilitated by copper enzymes and stabilized by multicopper oxidases. Herein, a nitrogen-doped copper sub-nanocluster catalyst (SNC) featured a high metal content (29.1 wt%) and uniform Cu distribution was synthesized by carbonizing the nanosheet-like metal–organic framework (MOF), enhancing bisphenol A degradation by activating peroxymonosulfate (PMS) to generate Cu(III). The degradation performance of the SNC outperformed the catalyst carbonized with the bulk-like MOF and matched the reported single-atom catalysts counterparts. Nitrogen doping decreased the electrons of Cu3d orbital, enhancing its bonding with the oxygen atom within the PMS molecule, thus promoting Cu(III) generation. The Cu-SNC/PMS system also showed robust resistance against anions, pH changes, and diverse water matrices. Importantly, it can selectively degrade electron-rich pollutants through oxygen atom transfer by Cu(III). This study provided new perspectives into SNC preparation, the controlled formation of high-valent metal species, and their role in Fenton-like reactions for pollutants degradation.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":null,"pages":null},"PeriodicalIF":8.1000,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"High metal-loaded sub-nanocluster catalyst enhanced Fenton-like reaction activity for emerging contaminants degradation by generating high-valent copper\",\"authors\":\"\",\"doi\":\"10.1016/j.seppur.2024.129794\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>High-valent copper (Cu(III)) species are crucial intermediates in C<img>H bond functionalization within both the biological and biomimetic processes, facilitated by copper enzymes and stabilized by multicopper oxidases. Herein, a nitrogen-doped copper sub-nanocluster catalyst (SNC) featured a high metal content (29.1 wt%) and uniform Cu distribution was synthesized by carbonizing the nanosheet-like metal–organic framework (MOF), enhancing bisphenol A degradation by activating peroxymonosulfate (PMS) to generate Cu(III). The degradation performance of the SNC outperformed the catalyst carbonized with the bulk-like MOF and matched the reported single-atom catalysts counterparts. Nitrogen doping decreased the electrons of Cu3d orbital, enhancing its bonding with the oxygen atom within the PMS molecule, thus promoting Cu(III) generation. The Cu-SNC/PMS system also showed robust resistance against anions, pH changes, and diverse water matrices. Importantly, it can selectively degrade electron-rich pollutants through oxygen atom transfer by Cu(III). This study provided new perspectives into SNC preparation, the controlled formation of high-valent metal species, and their role in Fenton-like reactions for pollutants degradation.</div></div>\",\"PeriodicalId\":427,\"journal\":{\"name\":\"Separation and Purification Technology\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":8.1000,\"publicationDate\":\"2024-09-20\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Separation and Purification Technology\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1383586624035330\",\"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":"Separation and Purification Technology","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1383586624035330","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}
High metal-loaded sub-nanocluster catalyst enhanced Fenton-like reaction activity for emerging contaminants degradation by generating high-valent copper
High-valent copper (Cu(III)) species are crucial intermediates in CH bond functionalization within both the biological and biomimetic processes, facilitated by copper enzymes and stabilized by multicopper oxidases. Herein, a nitrogen-doped copper sub-nanocluster catalyst (SNC) featured a high metal content (29.1 wt%) and uniform Cu distribution was synthesized by carbonizing the nanosheet-like metal–organic framework (MOF), enhancing bisphenol A degradation by activating peroxymonosulfate (PMS) to generate Cu(III). The degradation performance of the SNC outperformed the catalyst carbonized with the bulk-like MOF and matched the reported single-atom catalysts counterparts. Nitrogen doping decreased the electrons of Cu3d orbital, enhancing its bonding with the oxygen atom within the PMS molecule, thus promoting Cu(III) generation. The Cu-SNC/PMS system also showed robust resistance against anions, pH changes, and diverse water matrices. Importantly, it can selectively degrade electron-rich pollutants through oxygen atom transfer by Cu(III). This study provided new perspectives into SNC preparation, the controlled formation of high-valent metal species, and their role in Fenton-like reactions for pollutants degradation.
期刊介绍:
Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.