Lipeng Li , Xiuzhi Xu , Jin Wang, Jianjun Kang, Yan Chen, Fang Ke
{"title":"利用NiCl2@g-C3N4进行异相可见光光氧化催化,诱导C(sp2)-H/NH交叉脱氢偶联","authors":"Lipeng Li , Xiuzhi Xu , Jin Wang, Jianjun Kang, Yan Chen, Fang Ke","doi":"10.1016/j.mcat.2024.114633","DOIUrl":null,"url":null,"abstract":"<div><div>A novel photoactive NiCl<sub>2</sub>@g-C<sub>3</sub>N<sub>4</sub> catalyst system, which effectively drives C(sp<sup>2</sup>)-H/N<img>H bond formation between quinolin-2(1<em>H</em>)-ones, primary and secondary aliphatic amines under blue light irradiation. The NiCl<sub>2</sub>@g-C<sub>3</sub>N<sub>4</sub> composite with a NiCl<sub>2</sub> loading of 0.7wt% had the highest photoactivity, and the calculated band gap energy value is 2.56 eV The nickel ion could act as an electron acceptor enhancing carrier separation and transfer efficiency, greatly enhanced the photoreaction efficiency of g-C<sub>3</sub>N<sub>4</sub>. Preliminary mechanistic studies indicate upon visible light irradiation, the photo-generated electrons and holes act as oxidants, thereby generating amine radicals in the absence of external chemical oxidants. This provides a straightforward and efficient approach for directly 3-aminating quinoxalines-2(1<em>H</em>)-ones. Moreover, the heterogeneous catalyst can be recycled at least six times without significant activity loss.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"569 ","pages":"Article 114633"},"PeriodicalIF":3.9000,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Heterogeneous visible-light photoredox catalysis with NiCl2@g-C3N4 for induced C(sp2)-H/NH cross-dehydrogenative coupling\",\"authors\":\"Lipeng Li , Xiuzhi Xu , Jin Wang, Jianjun Kang, Yan Chen, Fang Ke\",\"doi\":\"10.1016/j.mcat.2024.114633\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>A novel photoactive NiCl<sub>2</sub>@g-C<sub>3</sub>N<sub>4</sub> catalyst system, which effectively drives C(sp<sup>2</sup>)-H/N<img>H bond formation between quinolin-2(1<em>H</em>)-ones, primary and secondary aliphatic amines under blue light irradiation. The NiCl<sub>2</sub>@g-C<sub>3</sub>N<sub>4</sub> composite with a NiCl<sub>2</sub> loading of 0.7wt% had the highest photoactivity, and the calculated band gap energy value is 2.56 eV The nickel ion could act as an electron acceptor enhancing carrier separation and transfer efficiency, greatly enhanced the photoreaction efficiency of g-C<sub>3</sub>N<sub>4</sub>. Preliminary mechanistic studies indicate upon visible light irradiation, the photo-generated electrons and holes act as oxidants, thereby generating amine radicals in the absence of external chemical oxidants. This provides a straightforward and efficient approach for directly 3-aminating quinoxalines-2(1<em>H</em>)-ones. Moreover, the heterogeneous catalyst can be recycled at least six times without significant activity loss.</div></div>\",\"PeriodicalId\":393,\"journal\":{\"name\":\"Molecular Catalysis\",\"volume\":\"569 \",\"pages\":\"Article 114633\"},\"PeriodicalIF\":3.9000,\"publicationDate\":\"2024-10-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Molecular Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2468823124008150\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Molecular Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2468823124008150","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Heterogeneous visible-light photoredox catalysis with NiCl2@g-C3N4 for induced C(sp2)-H/NH cross-dehydrogenative coupling
A novel photoactive NiCl2@g-C3N4 catalyst system, which effectively drives C(sp2)-H/NH bond formation between quinolin-2(1H)-ones, primary and secondary aliphatic amines under blue light irradiation. The NiCl2@g-C3N4 composite with a NiCl2 loading of 0.7wt% had the highest photoactivity, and the calculated band gap energy value is 2.56 eV The nickel ion could act as an electron acceptor enhancing carrier separation and transfer efficiency, greatly enhanced the photoreaction efficiency of g-C3N4. Preliminary mechanistic studies indicate upon visible light irradiation, the photo-generated electrons and holes act as oxidants, thereby generating amine radicals in the absence of external chemical oxidants. This provides a straightforward and efficient approach for directly 3-aminating quinoxalines-2(1H)-ones. Moreover, the heterogeneous catalyst can be recycled at least six times without significant activity loss.
期刊介绍:
Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are:
Heterogeneous catalysis including immobilized molecular catalysts
Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis
Photo- and electrochemistry
Theoretical aspects of catalysis analyzed by computational methods