���团簇催化剂在乙炔半加氢反应中的优异反应性

Acetylene semi-hydrogenation is a vital process where the utilization of supported isolated Pd atoms as catalytic active sites is promising due to their unique reactivity and metal atom efficacy. In particular, doping Pd single atoms at different sites on metal-oxide surfaces provides an opportunity to regulate their local coordination environments and modulate their electronic and catalytic properties. In this study, we conduct extensive density functional theory calculations to investigate the influence of single Pd atom coordination environments and surface properties on the activity and selectivity of Pd1/TiO2 catalysts for acetylene semi-hydrogenation. Considering the activity and selectivity, a four-atom single-cluster catalyst (SCC) of Pd1Ti3/TiO2 with negatively charged Pdδ− sites is found to exhibit excellent catalytic performance. Moreover, both activity and selectivity are highly correlated with the surface properties, including the d-band center index and surface work function. Our work provides theoretical guidance for the future design of heterogeneous SCC on reducible oxide supports for similar reactions in heterogeneous catalysis.