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

Abstract

Designing optimal heterogeneous metal hydrogenation catalysts for biomass conversion with simultaneously high activity and selectivity is a significant but challenging topic. Herein, we report a modularized hydrogenation mode with hydrogen dissociation and substrate activation on different sites (e.g., Pt and Cu), where Pt nanoclusters are responsible for H2 dissociation and Cu nanoparticles act as the active center for further substrate activation. Specifically, TS-1 zeolite@mesoporous silica with a core–shell structure was fabricated, in which the Pt and Cu species are confined within micropores and mesopores, respectively. Such configurations allow facile dissociation of H2 on Pt sites, followed by the migration of spilled-over hydrogen atoms to the Cu sites where the adsorbed substrates are activated for catalytic hydrogenation. This synergy yields an efficient furfural hydrogenation system with a high turnover frequency (32.8 h–1) and a remarkable furfuryl alcohol selectivity (>99.6%). The modularizing strategy opens up an innovative pathway for fabrication of hydrogenation catalysts with outstanding activity and high selectivity.