Mesoporous Ni–C hydrogenation catalysts with ultrafine Ni nanoparticles prepared via a phyllosilicate-assisted hard-templating strategy

Ni-phyllosilicate hard-templating yields sintering-resistant mesoporous Ni–C catalysts. • Achieves high-loading, ultrafine Ni NPs via a confined interfacial layer. • Enhanced SMSI and anti-leaching stability are confirmed by multi-technique analysis. • Superior LA-to-GVL hydrogenation: 99.7% conversion, 99.3% selectivity. • A general design for high-performance non-noble metal-carbon hydrogenation catalysts. Carbon-encapsulated metal catalysts prepared by in-situ carbonization generally suffer from severe metal sintering during high-temperature treatment. Herein, we develop a nickel phyllosilicate-assisted hard-templating strategy to construct mesoporous Ni–C catalysts with ultrafine, high-loading Ni nanoparticles partially embedded in the carbon support. A Ni 3 Si 2 O 5 (OH) 4 interfacial layer is pre-formed via ammonia evaporation prior to carbonization, which effectively inhibits Ni sintering and strengthens the metal-support interaction. The embedded structure generates charge-polarized Ni δ+ –Ni δ– sites that promote hydrogen dissociation and spillover, and enable synergistic activation of levulinic acid and H 2 . Under mild conditions (S/C = 50, 160 °C, 1 MPa H 2 ), the optimized Ni–C–p catalyst achieves 99.7% LA conversion and 99.3% γ-valerolactone selectivity within 2 h, with a reaction rate approximately three times that of conventional impregnated Ni/C. This strategy exhibits good universality for designing other non-noble metal-carbon composites toward challenging liquid-phase hydrogenation reactions. Download: Download high-res image (290KB) Download: Download full-size image