{"title":"电化学铜催化乙烯烯的不对称氰酯化反应。","authors":"Kehan Zhou,Niankai Fu","doi":"10.1038/s41467-025-62137-7","DOIUrl":null,"url":null,"abstract":"The heterodifunctionalization of alkenes is an efficient and straightforward method for the preparation of highly functionalized molecules. However, enantioselective introduction of two different carbon-based functional groups in a single step using readily accessible and inexpensive starting materials presents a significant challenge. Herein, we report an electrochemical copper-catalyzed protocol for the asymmetric cyanoesterification of vinylarenes using commercially available alkyl carbazates and trimethylsilyl cyanide (TMSCN) as the sources of ester and cyano groups, respectively. The desired products could be obtained with good yields and enantioselectivities under mild conditions without the need for stoichiometric oxidants, providing sustainable access to versatile synthetic intermediates that could be smoothly converted into a variety of useful chiral building blocks. Mechanistic data are consistent with electrochemical copper-catalyzed generation of alkoxycarbonyl radicals from alkyl carbazates and the copper catalyst is also responsible for the stereoselective C-CN bond formation. The potential synthetic utility of this new electrocatalytic protocol is demonstrated in the concise synthesis of pharmacologically active molecules.","PeriodicalId":19066,"journal":{"name":"Nature Communications","volume":"14 1","pages":"6767"},"PeriodicalIF":15.7000,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Asymmetric cyanoesterification of vinylarenes by electrochemical copper catalysis.\",\"authors\":\"Kehan Zhou,Niankai Fu\",\"doi\":\"10.1038/s41467-025-62137-7\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The heterodifunctionalization of alkenes is an efficient and straightforward method for the preparation of highly functionalized molecules. However, enantioselective introduction of two different carbon-based functional groups in a single step using readily accessible and inexpensive starting materials presents a significant challenge. Herein, we report an electrochemical copper-catalyzed protocol for the asymmetric cyanoesterification of vinylarenes using commercially available alkyl carbazates and trimethylsilyl cyanide (TMSCN) as the sources of ester and cyano groups, respectively. The desired products could be obtained with good yields and enantioselectivities under mild conditions without the need for stoichiometric oxidants, providing sustainable access to versatile synthetic intermediates that could be smoothly converted into a variety of useful chiral building blocks. Mechanistic data are consistent with electrochemical copper-catalyzed generation of alkoxycarbonyl radicals from alkyl carbazates and the copper catalyst is also responsible for the stereoselective C-CN bond formation. The potential synthetic utility of this new electrocatalytic protocol is demonstrated in the concise synthesis of pharmacologically active molecules.\",\"PeriodicalId\":19066,\"journal\":{\"name\":\"Nature Communications\",\"volume\":\"14 1\",\"pages\":\"6767\"},\"PeriodicalIF\":15.7000,\"publicationDate\":\"2025-07-23\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nature Communications\",\"FirstCategoryId\":\"103\",\"ListUrlMain\":\"https://doi.org/10.1038/s41467-025-62137-7\",\"RegionNum\":1,\"RegionCategory\":\"综合性期刊\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MULTIDISCIPLINARY SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature Communications","FirstCategoryId":"103","ListUrlMain":"https://doi.org/10.1038/s41467-025-62137-7","RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MULTIDISCIPLINARY SCIENCES","Score":null,"Total":0}
Asymmetric cyanoesterification of vinylarenes by electrochemical copper catalysis.
The heterodifunctionalization of alkenes is an efficient and straightforward method for the preparation of highly functionalized molecules. However, enantioselective introduction of two different carbon-based functional groups in a single step using readily accessible and inexpensive starting materials presents a significant challenge. Herein, we report an electrochemical copper-catalyzed protocol for the asymmetric cyanoesterification of vinylarenes using commercially available alkyl carbazates and trimethylsilyl cyanide (TMSCN) as the sources of ester and cyano groups, respectively. The desired products could be obtained with good yields and enantioselectivities under mild conditions without the need for stoichiometric oxidants, providing sustainable access to versatile synthetic intermediates that could be smoothly converted into a variety of useful chiral building blocks. Mechanistic data are consistent with electrochemical copper-catalyzed generation of alkoxycarbonyl radicals from alkyl carbazates and the copper catalyst is also responsible for the stereoselective C-CN bond formation. The potential synthetic utility of this new electrocatalytic protocol is demonstrated in the concise synthesis of pharmacologically active molecules.
期刊介绍:
Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.