Highly selective nickel-catalyzed gem-difluoropropargylation of unactivated alkylzinc reagents

被引:51
|
作者
An, Lun [1 ]
Xu, Chang [1 ]
Zhang, Xingang [1 ]
机构
[1] Univ Chinese Acad Sci, Chinese Acad Sci, Shanghai Inst Organ Chem, Key Lab Organofluorine Chem, 345 Lingling Rd, Shanghai 200032, Peoples R China
来源
NATURE COMMUNICATIONS | 2017年 / 8卷
基金
中国国家自然科学基金;
关键词
ARYL BORONIC ACIDS; CROSS-COUPLINGS; DIFLUOROMETHYLATED ARENES; SUBSTITUTION; PHEROMONE; BROMIDES; HALIDES; DIFLUOROALKYLATION; FLUOROALKYLATION; ELECTROPHILES;
D O I
10.1038/s41467-017-01540-1
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
In spite of the important applications of difluoroalkylated molecules in medicinal chemistry, to date, the reaction of difluoroalkylating reagents with unactivated, aliphatic substrates through a controllable manner remains challenging and has not been reported. Here we describe an efficient nickel-catalyzed cross-coupling of unactivated alkylzinc reagen\ts with gem-difluoropropargyl bromides. The reaction proceeds under mild reaction conditions with high efficiency and excellent regiochemical selectivity. Transformations of the resulting difluoroalkylated alkanes lead to a variety of biologically active molecules, providing a facile route for applications in drug discovery and development. Preliminary mechanistic studies reveal that an alkyl nickel intermediate [Ni(tpy)alkyl] (tpy, terpyridine) is involved in the catalytic cycle.
引用
收藏
页数:9
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