Silica‐Decoration Boosts Ni Catalysis for (De)hydrogenation: Step‐Abundant Nanostructures Stabilized by Silica

Ni nanoparticles supported on SiO2 were decorated with additional SiOx species by impregnation tetraethoxysilane (Si(OEt)4). The combination of electron microscopy, infrared analysis, and density functional theory (DFT) calculations revealed that the SiOx-decoration made surface morphology highly rough step-abundant due to significant stabilization low-coordination-number sites. SiOx-decorated exhibited 50 times higher catalytic activity for dehydrogenation methylcyclohexane toluene than pure Ni. DFT Ni(211) step sites had a more favorable C−H activation Ni(111) terrace well reproduced experimental apparent energies.