Rational Design of Pt–Co Synergy in Mesoscale Confinement: Enabling Stable C═O Selective Hydrogenation under Ambient Conditions

Developing efficient catalysts for selective C═O hydrogenation remains challenging due to the thermodynamic preference for C═C bond activation in α,β-unsaturated aldehydes. To address this limitation, we engineered Pt1Co10 nanoalloys within ethylenediamine-functionalized mesoporous silica (MS) by marrying vacuum-assisted impregnation with spatially constrained self-assembly. This dual spatial–temporal control strategy can achieve precise charge redistribution at metal interfaces, geometric confinement suppressing Ostwald ripening, and optimal hydrogenation pathways via hierarchical porosity. Under industry-feasible conditions (25 °C, 0.5 MPa H2), the Pt1Co10/MS system delivers 96.8% cinnamaldehyde conversion with 72.1% cinnamyl alcohol yield, outperforming conventional Pt or Co catalysts. More importantly, the MS framework’s strain accommodation capability enables activity retention over the cycle test, and the electronic synergy between Pt and Co can optimize adsorption energetics to suppress competitive C═C hydrogenation pathways. This work establishes an approach of bimetal synergy for steering adsorbed intermediate configurations, offering universal strategies for selective hydrogenation catalysis.