Zheng-Yan Huang, Jiayu Wei, P. Hu, Pu‐Cha Yan, Yuanqiang Li, Jian‐Hua Xie, Qi‐Lin Zhou
A series of 6-carbazole-modified Ir-SpiroPAP catalysts were designed for the asymmetric hydrogenation of indenones to chiral indenols. The optimized catalyst, featuring a 6-carbazole moiety on the pyridine ring and 3,5-dimethyl groups on the P -phenyl rings, achieved up to 98% yield, 95% ee, and an impressive turnover number (TON) of 7200. Density Functional Theory (DFT) analyses revealed that the 6-carbazole unit enhances catalyst rigidity, influencing enantioselectivity by inducing geometric distortion of the indenones during the hydrogenation process.