Methanol-Mediated Nickel-Catalyzed Chemo- and Enantioselective Three-Component Alkenylative Coupling of Aldimines and Alkynes with Alkenyl Boronic Acids

甲醇介导的镍催化醛亚胺和炔烃与烯基硼酸的化学选择性和对映选择性三组分烯基化偶联反应

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Abstract

1,3-Dienyl amines are important and versatile motifs in organic synthesis, and the functionalization of π-components with aldimines has emerged as a powerful strategy for their construction. However, existing methods typically rely on conjugated enynes or dienes and are limited to two-component reactions. Herein, we report a nickel-catalyzed chemoselective three-component alkenylative coupling of aldimines, simple alkynes, and alkenyl boronic acids, which provides stereodefined, multisubstituted 1,3-dienyl amines in good to excellent yields (up to 97% yield). Methanol acts as a sustainable protic solvent, facilitating the ring opening of the aza-nickelacycle intermediate generated via oxidative cyclization of the aldimine and alkyne. Furthermore, employing a P-chiral monophosphine ligand allows the enantioselective variant of this reaction to proceed with excellent stereocontrol (up to 98% yield and 99% ee).

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