Porous graphene-assisted dynamic Pd catalysis for superior hydrogenation

Statically immobilized Pd active sites leads to suboptimal hydrogenation efficacy even under harsh reaction conditions, and dynamic catalysis for individual requirements of H-2 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 degrees C 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.