Ultrahigh Selective Hydrogenation of Furfural Enabled by Modularizing Hydrogen Dissociation and Substrate Activation

Designing optimal heterogeneous metal hydrogenation catalystsforbiomass conversion with simultaneously high activity and selectivityis a significant but challenging topic. Herein, we report a modularizedhydrogenation mode with hydrogen dissociation and substrate activationon different sites (e.g., Pt and Cu), where Pt nanoclusters are responsiblefor H-2 dissociation and Cu nanoparticles act as the activecenter for further substrate activation. Specifically, TS-1 zeolite@mesoporoussilica with a core-shell structure was fabricated, in whichthe Pt and Cu species are confined within micropores and mesopores,respectively. Such configurations allow facile dissociation of H-2 on Pt sites, followed by the migration of spilled-over hydrogenatoms to the Cu sites where the adsorbed substrates are activatedfor catalytic hydrogenation. This synergy yields an efficient furfuralhydrogenation system with a high turnover frequency (32.8 h(-1)) and a remarkable furfuryl alcohol selectivity (>99.6%). Themodularizingstrategy opens up an innovative pathway for fabrication of hydrogenationcatalysts with outstanding activity and high selectivity.