Atomically Precise Defective Copper Nanocluster Catalysts for Highly Selective C−C Cross‐Coupling Reactions

Abstract Point defects in nanoparticles have long been hypothesized to play an important role in governing the particle's electronic structure and physicochemical properties. However, single point defects in material systems usually exist with other heterogeneities, obscuring the chemical role of the effects. Herein, we report the synthesis of novel atomically precise, copper hydride nanoclusters (NCs), [Cu 28 H 10 (C 7 H 7 S) 18 (TPP) 3 ] ( Cu 28 ; TPP: triphenylphosphine; C 7 H 7 S: o ‐thiocresol) with a defined defect in the gram scale via a one‐pot reduction method. The Cu 28 acts as a highly selective catalyst for C−C cross‐couplings. The work highlights the potential of defective NCs as model systems for investigating individual defects, correlating defects with physiochemical properties, and rationally designing new nanoparticle catalysts.