催化作用
钴
化学
简单(哲学)
赫克反应
钯
组合化学
有机化学
认识论
哲学
作者
Chunyang Zhao,Chao Dong,Wenxuan Ma,Lili Shi,Dezhi Liu,Xiaoxuan Zhang,Zhoufeng Cui,Zhiwei Wang,Junkai Fu
出处
期刊:ACS Catalysis
[American Chemical Society]
日期:2024-09-16
卷期号:14 (19): 14475-14485
被引量:7
标识
DOI:10.1021/acscatal.4c03917
摘要
Regiocontrol has been a long-standing challenge in the Heck-type reaction of unactivated alkenes due to the presence of multiple detachable β-hydrogens, but it also represents an intriguing research topic owing to the potential for accessing structurally diverse internal aliphatic alkenes. Herein, a cobalt-catalyzed regiodivergent Heck-type reaction of simple unactivated alkenes and fluoroalkyl bromides is reported, yielding a variety of internal aliphatic olefins containing biologically relevant fluorinated moieties. This directing-group-free protocol shows a broad substrate scope encompassing terminal, 1,1-disubstituted, and internal alkenes, as well as di-, per-, and monofluoroalkyl bromides, and exhibits a good functional group tolerance even toward unprotected polar functionalities. Mechanistic investigations reveal a portfolio strategy involving an initial atom transfer radical addition (ATRA) process followed by a remarkably tunable site-selective H–Br elimination, leading to either vinyl or contra-thermodynamic allylic Heck-type products based on the presence of different external additives.
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