Huang Nan, Luo Jie, Liao Lihao, Zhao Xiaodan
Institute of Organic Chemistry and MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, IGCME, Sun Yat-Sen University, Guangzhou 510006, China.
J Am Chem Soc. 2024 Mar 13;146(10):7029-7038. doi: 10.1021/jacs.4c00307. Epub 2024 Mar 1.
Enantioselective difunctionalization of alkenes offers a straightforward means for the rapid construction of enantioenriched complex molecules. Despite the tremendous efforts devoted to this field, enantioselective aminative difunctionalization remains a challenge, particularly through an electrophilic addition fashion. Herein, we report an unprecedented approach for the enantioselective aminative difunctionalization of alkenes via copper-catalyzed electrophilic addition with external azo compounds as nitrogen sources. A series of valuable cyclic hydrazine derivatives via either [3 + 2] cycloaddition or intramolecular cyclization have been achieved in high chemo-, regio-, enantio-, and diastereoselectivities. In this transformation, a wide range of functional groups, such as carboxylic acid, hydroxy, amide, sulfonamide, and aryl groups, could serve as nucleophiles. Importantly, a new cyano oxazoline chiral ligand was found to play a crucial role in the control of enantioselectivity.
烯烃的对映选择性双官能化反应为快速构建对映体富集的复杂分子提供了一种直接的方法。尽管在该领域已付出巨大努力,但对映选择性胺化双官能化反应仍然是一项挑战,特别是通过亲电加成方式。在此,我们报道了一种前所未有的方法,通过铜催化以外部偶氮化合物作为氮源的亲电加成反应实现烯烃的对映选择性胺化双官能化。通过[3 + 2]环加成或分子内环化反应,已以高化学、区域、对映和非对映选择性得到了一系列有价值的环状肼衍生物。在该转化反应中,多种官能团,如羧酸、羟基、酰胺、磺酰胺和芳基等,均可作为亲核试剂。重要的是,发现一种新型氰基恶唑啉手性配体在对映选择性控制中起着关键作用。