Wang, Shou‐GuoLiu, YangCramer, Nicolai2021-01-252021-01-252021-01-252019-09-2510.1002/anie.201909971https://infoscience.epfl.ch/handle/20.500.14299/174928An efficient CpxRhIII‐catalyzed enantioselective alkenyl C−H functionalization/[4+1] annulation of acryl amides and allenes is reported. The described transformation provides straightforward access to enantioenriched α,β‐unsaturated‐γ‐lactams bearing a quaternary stereocenter. The reaction operates under mild conditions, displays a broad functional‐group tolerance, and provides 2H‐pyrrol‐2‐ones with excellent selectivity of up to 97:3 er. Such scaffolds are frequently found in natural products and synthetic bioactive compounds and are of significant synthetic value. It is noteworthy that the allene serves as a one‐carbon unit in the [4+1]‐annulation.Asymmetric Alkenyl C−H Functionalization by Cp x Rh III forms 2 H ‐Pyrrol‐2‐ones through [4+1]‐Annulation of Acryl Amides and Allenestext::journal::journal article::research article