摘要
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 CO_(2)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.
基金
This work was financially supported by the National Natural Science Foundation of China(grant no.22033005 to J.L.and grant no.21903047 to H.X.)
The support of Guangdong Provincial Key Laboratory of Catalysis(grant no.2020B121201002)is also acknowledged.The calculations were performed using the supercomputers at Tsinghua National Laboratory for Information Science and Technology,the Computational Chemistry Laboratory of the Department of Chemistry under the Tsinghua Xuetang Talents Program,and the Supercomputer Center of the Southern University of Science and Technology.
