Li Xiangdong, Waser Jérôme
Laboratory of Catalysis and Organic Synthesis, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Fédérale de Lausanne, Lausanne CH-1015, Switzerland.
J Am Chem Soc. 2024 Oct 30;146(43):29712-29719. doi: 10.1021/jacs.4c10996. Epub 2024 Oct 18.
1,1'-Bicyclopropenyl is a constitutional isomer of benzene comprising two coupled cyclopropene units with the endocyclic double bonds in conjugation. Due to the intrinsic high strain energy, it remains a long-standing challenge to prepare 1,1'-bicyclopropenyl derivatives, particularly multisubstituted, nonsymmetrical ones, in an efficient and modular manner. Herein a straightforward Au/Ag bimetallic-catalyzed cyclopropenyl cross-coupling has been developed, providing a robust and versatile strategy for the rapid assembly of symmetrical and unsymmetrical 1,1'-bicyclopropenyl derivatives from cyclopropenyl benziodoxoles (CpBXs) and terminal cyclopropenes. Advantages of this strategy include tolerance to a wide range of synthetically useful functional groups, mild reaction conditions, and a simple catalytic system. The obtained 1,1'-bicyclopropenyl derivatives were shown to be valuable synthetic intermediates through selective downstream manipulations.
1,1'-双环丙烯基是苯的一种构造异构体,由两个相连的环丙烯单元组成,其环内双键共轭。由于其固有的高应变能,以高效且模块化的方式制备1,1'-双环丙烯基衍生物,特别是多取代、不对称的衍生物,仍然是一个长期存在的挑战。在此,已开发出一种直接的金/银双金属催化的环丙烯基交叉偶联反应,为从环丙烯基苯碘酰(CpBXs)和末端环丙烯快速组装对称和不对称的1,1'-双环丙烯基衍生物提供了一种强大且通用的策略。该策略的优点包括对多种具有合成用途的官能团具有耐受性、反应条件温和以及催化体系简单。通过选择性的下游操作,所得到的1,1'-双环丙烯基衍生物被证明是有价值的合成中间体。