{"title":"铜催化苯乙烯与烷烃和酰胺的对映选择性三组分羧酰胺化反应","authors":"Ying-Ying Chen, Ling Dai, Xuan-Ge Zhang, Qi-Lin Zhou","doi":"10.1021/jacs.5c02348","DOIUrl":null,"url":null,"abstract":"Efficient assembly of valuable chiral molecules from readily available and low-cost chemical feedstocks remains one of the most challenging tasks in synthetic chemistry today. Radical-mediated three-component carboamination of alkenes offers an attractive strategy for addressing this challenge. However, most existing reports focus on racemic examples and are largely limited to activated alkenes, preactivated alkylation reagents, or sufficiently active nucleophiles. Herein, we report a highly enantioselective three-component carboamidation of styrenes with unactivated alkanes and weakly nucleophilic amides. Enantioselective control is achieved by using chiral cationic copper catalysts. This method enables the synthesis of a variety of optically active amides with excellent enantioselectivity. Mechanistic studies reveal that the reaction proceeds via hydrogen atom transfer from the alkane followed by radical addition to the olefin.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"63 1","pages":""},"PeriodicalIF":15.6000,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Copper-Catalyzed Enantioselective Three-Component Carboamidation of Styrenes with Alkanes and Amides\",\"authors\":\"Ying-Ying Chen, Ling Dai, Xuan-Ge Zhang, Qi-Lin Zhou\",\"doi\":\"10.1021/jacs.5c02348\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Efficient assembly of valuable chiral molecules from readily available and low-cost chemical feedstocks remains one of the most challenging tasks in synthetic chemistry today. Radical-mediated three-component carboamination of alkenes offers an attractive strategy for addressing this challenge. However, most existing reports focus on racemic examples and are largely limited to activated alkenes, preactivated alkylation reagents, or sufficiently active nucleophiles. Herein, we report a highly enantioselective three-component carboamidation of styrenes with unactivated alkanes and weakly nucleophilic amides. Enantioselective control is achieved by using chiral cationic copper catalysts. This method enables the synthesis of a variety of optically active amides with excellent enantioselectivity. Mechanistic studies reveal that the reaction proceeds via hydrogen atom transfer from the alkane followed by radical addition to the olefin.\",\"PeriodicalId\":49,\"journal\":{\"name\":\"Journal of the American Chemical Society\",\"volume\":\"63 1\",\"pages\":\"\"},\"PeriodicalIF\":15.6000,\"publicationDate\":\"2025-04-04\",\"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.5c02348\",\"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.5c02348","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Copper-Catalyzed Enantioselective Three-Component Carboamidation of Styrenes with Alkanes and Amides
Efficient assembly of valuable chiral molecules from readily available and low-cost chemical feedstocks remains one of the most challenging tasks in synthetic chemistry today. Radical-mediated three-component carboamination of alkenes offers an attractive strategy for addressing this challenge. However, most existing reports focus on racemic examples and are largely limited to activated alkenes, preactivated alkylation reagents, or sufficiently active nucleophiles. Herein, we report a highly enantioselective three-component carboamidation of styrenes with unactivated alkanes and weakly nucleophilic amides. Enantioselective control is achieved by using chiral cationic copper catalysts. This method enables the synthesis of a variety of optically active amides with excellent enantioselectivity. Mechanistic studies reveal that the reaction proceeds via hydrogen atom transfer from the alkane followed by radical addition to the olefin.
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.