{"title":"通过铝-硅合作实现亚硝基炔的多电子还原","authors":"Xi Chen, Dezhi Yang, Fanshu Cao, Zhenbo Mo","doi":"10.1021/jacs.4c10323","DOIUrl":null,"url":null,"abstract":"The cooperative effects of main-group elements pave the way for novel chemical transformations. However, the potential of bimetallic complexes featuring the most abundant aluminum and silicon elements remains largely unexplored. In this study, we present the synthesis and characterization of bis(silylene)-stabilized aluminylene <b>2</b>. The cooperation between aluminylene and silylene allows for the facile cleavage of the N–O bond in nitrosoarenes, producing an aluminum imide complex <b>4</b> and tetracyclic oxazasilaalanes <b>5</b> and <b>6</b>, and also promotes the dearomatization of 2-methylquinoline, yielding a silylalane <b>7</b>. In addition, <b>2</b> is an effective precatalyst for the reductive coupling of nitrosoarenes to azoxyarenes. These results outline an approach for orchestrating aluminum and silicon cooperation to facilitate chemical bond activation.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":null,"pages":null},"PeriodicalIF":14.4000,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Multielectron Reduction of Nitrosoarene via Aluminylene-Silylene Cooperation\",\"authors\":\"Xi Chen, Dezhi Yang, Fanshu Cao, Zhenbo Mo\",\"doi\":\"10.1021/jacs.4c10323\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The cooperative effects of main-group elements pave the way for novel chemical transformations. However, the potential of bimetallic complexes featuring the most abundant aluminum and silicon elements remains largely unexplored. In this study, we present the synthesis and characterization of bis(silylene)-stabilized aluminylene <b>2</b>. The cooperation between aluminylene and silylene allows for the facile cleavage of the N–O bond in nitrosoarenes, producing an aluminum imide complex <b>4</b> and tetracyclic oxazasilaalanes <b>5</b> and <b>6</b>, and also promotes the dearomatization of 2-methylquinoline, yielding a silylalane <b>7</b>. In addition, <b>2</b> is an effective precatalyst for the reductive coupling of nitrosoarenes to azoxyarenes. These results outline an approach for orchestrating aluminum and silicon cooperation to facilitate chemical bond activation.\",\"PeriodicalId\":49,\"journal\":{\"name\":\"Journal of the American Chemical Society\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":14.4000,\"publicationDate\":\"2024-10-17\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of the American Chemical Society\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/jacs.4c10323\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the American Chemical Society","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/jacs.4c10323","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Multielectron Reduction of Nitrosoarene via Aluminylene-Silylene Cooperation
The cooperative effects of main-group elements pave the way for novel chemical transformations. However, the potential of bimetallic complexes featuring the most abundant aluminum and silicon elements remains largely unexplored. In this study, we present the synthesis and characterization of bis(silylene)-stabilized aluminylene 2. The cooperation between aluminylene and silylene allows for the facile cleavage of the N–O bond in nitrosoarenes, producing an aluminum imide complex 4 and tetracyclic oxazasilaalanes 5 and 6, and also promotes the dearomatization of 2-methylquinoline, yielding a silylalane 7. In addition, 2 is an effective precatalyst for the reductive coupling of nitrosoarenes to azoxyarenes. These results outline an approach for orchestrating aluminum and silicon cooperation to facilitate chemical bond activation.
期刊介绍:
The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.