Pd single-atom catalysts derived from strong metal-support interaction for selective hydrogenation of acetylene

Abstract

Selective hydrogenation of acetylene in excess ethylene is an important reaction in both fundamental study and practical application. Pd-based catalysts with high intrinsic activity are commonly employed, but usually suffer from low selectivity. Pd single-atom catalysts (SACs) usually exhibit outstanding ethylene selectivity due to the weak pi-bonding ethylene adsorption. However, the preparation of high-loading and stable Pd SACs is still confronted with a great challenge. In this work, we report a simple strategy to fabricate Pd SACs by means of reducing conventional supported Pd catalysts at suitable temperatures to selectively encapsulate the co-existed Pd nanoparticles (NPs)/clusters. This is based on our new finding that single atoms only manifest strong metal-support interaction (SMSI) at higher reduction temperature than that of NPs/clusters. The derived Pd SACs (Pd-1/CeO2 and Pd-1/alpha-Fe2O3) were applied to acetylene selective hydrogenation, exhibiting much improved ethylene selectivity and high stability. This work offers a promising way to develop stable Pd SACs easily.