• A porous carbon-supported Ni-ZnO nanoparticles catalyst (Ni-ZnO/AC) was synthesized by low-temperature coprecipitation, demonstrating exceptional catalytic activity and stability.
• Selective hydrogenation of 5-hydroxymethylfurfural (HMF) to 2,5-bis(hydroxymethyl)furan (97.5%) or 2,5-dimethylfuran (99.5%) is achieved over Ni-ZnO/AC catalyst by solvent-tuning.
• Solvent-catalyst interaction jointly regulates hydrodeoxygenation behavior in HMF hydrogenation by modulating rate and pathway via a hydrogen shuttle mechanism.
• Density functional theory calculations confirm a lower activation energy in isopropanol (0.60 eV) compared to 1,4-dioxane (1.07 eV), providing mechanistic insights for solvent-mediated control.