Liu Jian-Guo, Zhang Wen-Ping, Xu Ming-Hua
Shenzhen Grubbs Institute and Department of Chemistry, Southern University of Science and Technology, 1088 Xueyuan Boulevard, Shenzhen 518055, China.
School of Chemistry and Chemical Engineering, Henan Normal University, Xinxiang 453007, Henan, China.
J Am Chem Soc. 2025 Sep 17;147(37):33691-33699. doi: 10.1021/jacs.5c09400. Epub 2025 Aug 22.
Despite notable progress in the study of chiral boron compounds, research on tetracoordinate chiral boron species remains limited. Achieving a configurationally stable boron stereocenter typically requires stabilizing the tetrahedral structure of the boron atom with suitable Lewis bases. Moreover, due to the high reactivity of borane complexes and the limited methods for their modification, designing and synthesizing tetracoordinate chiral boron compounds with stable stereocenters presents considerable challenges. Herein, we report the use of prochiral NHC carbene-substituted boranes in rhodium(I)/chiral diene and copper(I)/chiral bisoxazoline-catalyzed systems, achieving the stereodivergent synthesis of organoboron compounds featuring contiguous carbon and boron stereocenters via enantioselective desymmetrization of carbene B-H insertion. Both catalytic systems delivered good yields and high stereoselectivity (up to 99% ee and 93:7 dr), allowing access to the full complement of stereoisomers at will. Structural analysis of the typical product revealed a tetrahedral character of 91.1% for the boron stereocenters, demonstrating their high configurational stability. This work provides a robust approach to accessing structurally diverse and configurationally stable tetracoordinate chiral boron compounds.
尽管在手性硼化合物的研究方面取得了显著进展,但对四配位手性硼物种的研究仍然有限。实现构型稳定的硼立体中心通常需要用合适的路易斯碱来稳定硼原子的四面体结构。此外,由于硼烷配合物的高反应活性以及其修饰方法有限,设计和合成具有稳定立体中心的四配位手性硼化合物面临着相当大的挑战。在此,我们报道了在手性铑(I)/手性二烯和铜(I)/手性双恶唑啉催化体系中使用前手性NHC卡宾取代的硼烷,通过卡宾硼氢键插入的对映选择性去对称化实现了具有相邻碳和硼立体中心的有机硼化合物的立体发散合成。两种催化体系都能提供良好的产率和高立体选择性(高达99% ee和93:7 dr),从而能够随意获得所有立体异构体。对典型产物的结构分析表明,硼立体中心的四面体特征为91.1%,证明了它们具有高构型稳定性。这项工作为获得结构多样且构型稳定的四配位手性硼化合物提供了一种可靠的方法。