Chiral Magnesium Bisphosphate-Catalyzed Asymmetric Double C(sp³)–H Bond Functionalization Based on Sequential Hydride Shift/Cyclization Process

Described herein is a chiral magnesium bisphosphate-catalyzed asymmetric double C­(sp3)–H bond functionalization triggered by a sequential hydride shift/​cyclization process. This reaction consists of stereo­selective domino C­(sp3)–H bond functionalization: (1) a highly enantio- and diastereo­selective C­(sp3)–H bond functionalization by chiral magnesium bisphosphate (first [1,5]-hydride shift), and (2) a highly diastereo­selective C­(sp3)–H bond functionalization by an achiral catalyst (Yb­(OTf)3, second [1,5]-hydride shift).