电化学铜催化乙烯烯的不对称氰酯化反应。

IF 15.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Kehan Zhou,Niankai Fu
{"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}
引用次数: 0

摘要

烯烃的杂化双官能化是制备高官能化分子的一种简便有效的方法。然而,使用易于获取且价格低廉的起始材料在一个步骤中对映选择性地引入两个不同的碳基官能团是一个重大的挑战。本文报道了一种电化学铜催化乙烯烯不对称氰基酯化反应的方案,分别使用市售的烷基氨基甲酸酯和三甲基硅基氰化物(TMSCN)作为酯和氰基的来源。在温和的条件下,在不需要化学计量氧化剂的情况下,可以以良好的产率和对映选择性获得所需的产品,为多功能合成中间体提供了可持续的途径,这些中间体可以顺利地转化为各种有用的手性构建块。机制数据与电化学铜催化烷基氨基甲酸酯生成烷氧羰基自由基一致,铜催化剂也负责立体选择性C-CN键的形成。这种新的电催化方案的潜在的合成用途是在简洁的合成药理学活性分子。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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.
求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
Nature Communications
Nature Communications Biological Science Disciplines-
CiteScore
24.90
自引率
2.40%
发文量
6928
审稿时长
3.7 months
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.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术官方微信