马尔科夫尼科夫法则
催化作用
钴
化学
对偶(语法数字)
双重角色
有机化学
组合化学
光化学
区域选择性
文学类
艺术
作者
Arman Khosravi,Yu Zhang,Gaoyuan Zhao,Kelton Radefeld,Sahil Sharma,Nuwan Pannilawithana,Yuxiang Zhang,Peng Liu,Ming‐Yu Ngai
标识
DOI:10.26434/chemrxiv-2025-2nrb8
摘要
Alkyl halides are ubiquitous motifs in pharmaceuticals, agrochemicals, and materials, yet direct access to regioisomeric variants re-mains limited. Conventional hydrohalogenation of alkenes proceeds via ionic or radical pathways and is generally confined to 1,2-addition. Here, we report a dual cobalt/photoredox catalytic platform that enables remote-Markovnikov-selective 1,3-hydrobromination and hydrochlorination of allyl carboxylates. The transformation proceeds via a metal–hydride hydrogen atom transfer (MHAT) from a Co–H species, 1,2-radical acyloxy migration (1,2-RAM), and halogen atom transfer (XAT) from a Co–X complex. This strategy delivers β-acyloxy alkyl halides under mild conditions, with broad functional group tolerance, compatibility with complex molecules, and scalability. Mechanistic experiments support a radical relay sequence that diverges from classical regi-oselectivity to access formal 1,3-addition products. This work establishes a general approach to regioselective C–X bond formation via programmable radical migration and expands the synthetic toolbox for alkene hydrofunctionalization.
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