Zou Jian-Yu, Xing Fang-Li, Zi Quan-Xing, Du Hai-Wu, Chen Meiwan, Shu Wei
Shenzhen Key Laboratory of Small Molecule Drug Discovery and Synthesis, Shenzhen Grubbs Institute, Guangming Advanced Research Institute, Department of Chemistry, and Guangdong Provincial Key Laboratory of Catalysis, Southern University of Science and Technology, Shenzhen 518055, Guangdong, P. R. China.
State Key Laboratory of Quality Research in Chinese Medicine, Institute of Chinese Medical Sciences, University of Macau, Macau SAR, P. R. China.
Sci Adv. 2025 Jun 13;11(24):eadv6571. doi: 10.1126/sciadv.adv6571.
α-Chiral phosphorus compounds have broad applications as organic catalysts or ligands in organic chemistry and related areas. Herein, we disclose a Ni-catalyzed enantioselective cross-hydrodimerization of alkenyl phosphine sulfides with unactivated alkenes to access α-chiral phosphine sulfides, representing the first example of asymmetric hydrodimerization of electron-deficient alkenes with electron-rich alkenes. Key to success is the precise recognition between electron-deficient alkenes and electron-rich alkenes and streamlined alkyl-alkyl bond forming with the control of chemo-, regio-, and enantioselectivity. This strategy requires alkenes as sole precursors for asymmetric alkyl-alkyl cross-coupling, circumventing the use of stoichiometric amounts of alkyl electrophiles or alkyl nucleophiles as coupling partners. The mild conditions tolerate a wide range of functional groups, providing direct access to α-chiral phosphines through a carbon-carbon bond-forming process without prefunctionalized coupling precursors.
α-手性磷化合物作为有机催化剂或配体在有机化学及相关领域有着广泛的应用。在此,我们报道了一种镍催化的链烯基膦硫化物与未活化烯烃的对映选择性交叉氢二聚反应,以制备α-手性膦硫化物,这是缺电子烯烃与富电子烯烃不对称氢二聚反应的首例。成功的关键在于缺电子烯烃与富电子烯烃之间的精确识别,以及通过化学、区域和对映选择性控制实现简化的烷基-烷基键形成。该策略要求烯烃作为不对称烷基-烷基交叉偶联的唯一前体,避免使用化学计量的烷基亲电试剂或烷基亲核试剂作为偶联伙伴。温和的反应条件能容忍多种官能团,通过碳-碳键形成过程直接制备α-手性膦,无需预官能化的偶联前体。