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 °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 (PdN 4) 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 PdN 4 and Pd NPs. Importantly, All-in-one system is applicable for complex bio–oil hydrogenation and for a broad spectrum of unsaturated substrates. [Display omitted] • The dynamic Pd catalysis assisted by porous graphene has superior hydrogenation activity. • The All-in-one system integrates catalyst preparation and substrate conversion. • The excellent activity comes from the synergistic effects of PdN 4 and Pd NPs. • Proposing a green strategy for bio-based chemicals production or bio-oil upgrading. [ABSTRACT FROM AUTHOR]