Litcius/Paper detail

NiH-Catalyzed Homobenzylic Hydroalkylation of Aryl Alkenes Using Sulfoxonium Ylides

Qing Wang, Hoonchul Choi, Xiang Lyu, Dongwook Kim, Sukbok Chang

2025Journal of the American Chemical Society5 citationsDOI

Abstract

We present here the first example of NiH-catalyzed homobenzylic hydroalkylation of aryl alkenes mediated by a nickel carbene radical, achieving the elusive β-selectivity with excellent regiocontrol. Mechanistic investigations suggest that this transformation is enabled by the preferential engagement of NiH with bench-stable sulfoxonium ylides, whose unique chelation properties promote carbene activation prior to alkene insertion. The resulting nickel carbene radical is proposed to undergo selective β-addition, followed by intramolecular metal hydride transfer and protodemetalation. The reaction exhibits broad scope across aryl, heteroaryl, and complex bioactive alkene derivatives, as well as diverse sulfoxonium ylides. This work establishes a new mechanistic platform for NiH catalysis, expanding the synthetic repertoire for site-selective alkene functionalization.

Topics & Concepts

ChemistryAlkeneCarbeneArylIntramolecular forceCombinatorial chemistryHydrideNickelScope (computer science)Organic chemistryRadicalCatalytic C–H Functionalization MethodsCyclopropane Reaction MechanismsAsymmetric Hydrogenation and Catalysis