Porous Graphene-Assisted Dynamic Pd Catalysis for Superior Hydrogenation

Abstract

Statically immobilized Pd active sites leads to suboptimal hydrogenation efficacy even under harsh reaction conditions, and dynamic catalysis for individual requirements of H2 dissociation and substrate activation is devoid. Here, we have developed an innovative All-in-one system that employs dynamic Pd catalysis assisted by porous graphene, enabling hydrogenation to be conducted under mild conditions. The conversion of vanillin at 30 oC is 99% and the yield of 2-methoxy-4-methylphenol is >95%, significantly exceeding the reported records. The uniformly distributed N-doping and thin sheets of porous graphene induce Pd single-atom (PdN4) formation, and inhibit rapid agglomeration to nanoparticles (Pd NPs) for assisting dynamic catalysis. High pressure process analysis and theoretical calculations reveal that excellent activity comes from the synergistic effects of PdN4 and Pd NPs. Importantly, All-in-one system is applicable for complex bio–oil hydrogenation and for a broad spectrum of unsaturated substrates.

Keywords: Porous graphene, Hydrogenation, The All-in-one system, Dynamic Pd catalysis