Highly Selective Dual-Atom Pd Heterogeneous Catalyst Prepared by Size-Selected Cluster Beam

Abstract

Atomic dispersed heterogeneous catalysts have emerged as a prominent research focus in catalysis due to their exceptional atom utilization, robust activity, and remarkable selectivity. However, the design and synthesis of catalysts with a precisely defined atomic number and exceptional dispersion still pose significant challenges. In this study, we employed a magnetron sputtering cluster source equipped with a mass selector to selectively fabricate single-atom, dual-atom, and clusters with precise atomic numbers catalysts supported on mesoporous graphitic carbon nitride (mpg-C3N4). This method provides a universally applicable approach for synthesizing highly pure diatomic catalysts. Furthermore, the dual-atom Pd catalyst exhibits an outstanding turnover frequency of 5819 h–1 in the hydrogenation of nitrobenzene, surpassing that of both single-atom Pd and Pd2057 clusters. Density functional theory calculations reveal that excellent hydrogenation performance benefits from the easier dissociation of H–H bonds at the atomic geminal Pd2 sites in the hydrogenation process of nitrobenzene compared to that of single-atom Pd and Pd clusters. This work presents a universal synthetic strategy for precisely constructing multimetal atomic centers, showcasing the advantages of geminal metal sites in catalyzing multimolecule-involved reactions.