Litcius/Paper detail

Nitrene transfer from a sterically confined copper nitrenoid dipyrrin complex

Kurtis M. Carsch, Sasha C. North, Ida M. DiMucci, Andrei Iliescu, Petra Vojáčková, Thomas Khazanov, Shao‐Liang Zheng, Thomas R. Cundari, Kyle M. Lancaster, Theodore A. Betley

2023Chemical Science19 citationsDOIOpen Access PDF

Abstract

) and parallel kinetic isotope effect measurements (1.10(2)) are consistent with rate-limiting Cu nitrenoid formation, followed by a proposed stepwise hydrogen-atom abstraction and rapid radical recombination to furnish the resulting C-N bond. The proposed mechanism and experimental analysis are further corroborated by density functional theory calculations. Multiconfigurational calculations provide insight into the electronic structure of the catalytically relevant Cu nitrene intermediates. The findings presented herein will assist in the development of future methodology for Cu-mediated C-N bond forming catalysis.

Topics & Concepts

NitreneChemistryCopperSteric effectsAminationAdductPhotochemistryCombinatorial chemistryPolymer chemistryStereochemistryOrganic chemistryCatalysisSynthesis and Catalytic ReactionsPharmacological Receptor Mechanisms and EffectsMetal-Catalyzed Oxygenation Mechanisms