Electronic perturbation-promoted interfacial pathway for facile C–H dissociation

Abstract

Interface has often played significant role in the behavior of metal-based catalysts during various heterogeneous reactions. Herein, we reported a novel interfacial pathway for propane dehydrogenation on Pt-GaOx dual sites. The active ensemble, composing Pt particles and Ga2O3 clusters, facilitates the facile dissociation of C–H bonds (energy barrier < 0.30 eV) through H-abstraction by O sites, coupled with alkyl stabilization on the Pt surface. Notably, the electronic perturbation of the Pt slab induces higher-lying O 2p states at the interface, accompanied by a substantial density of states around fermi level. This is in stark contrast to the O species present in Ga2O3 crystals or clusters alone, leading to an exceptionally strong affinity for H and a robust ability for C–H scission. The Pt/Ga-Al2O3 catalysts prepared with Pt nanoparticles decorated by Ga oxide exhibit superior performance compared to Pt/Al2O3 and PtSn/Al2O3 catalysts. This insight into interfacial catalysis contributes to a broader understanding of the origin of the high catalytic efficiency observed in metal-based catalysts.