Computational Prediction of Graphdiyne-Supported Three-Atom Single-Cluster Catalysts

Abstract

While heterogeneous single-atom catalysts (SACs) have achieved great success in the past decade, their application is potentially limited by their simplistic single-atom active centers, which make single-cluster catalysts (SCCs) a natural extension in the domain of heterogeneous catalysis. SCCs with precise numbers of atoms and structural configurations possess SAC merits, yet have greater potential for catalyzing complex reactions and/or bulky reactants. Through systematic quantum-chemical studies and computational screening, we report here the rational design of transition metal three-atom clusters anchored on graphdiyne (GDY) as a novel kind of stable SCC with great promise for efficient and atomically precise heterogenous catalysis. By investigating their structure and catalytic performance for the oxygen reduction reaction, the hydrogen evolution reaction, and the CO2 reduction reaction, we have provided theoretical guidelines for their potential applications as heterogeneous catalysts. These GDY-supported three-atom SCCs provide an ideal benchmark scaffold for rational design of atomically precise heterogeneous catalysts for industrially important chemical reactions. (Figure Presented)