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

Abstract Ni nanoparticles supported on SiO 2 were decorated with additional SiO x species by impregnation with tetraethoxysilane (Si(OEt) 4 ). The combination of electron microscopy, infrared analysis, and density functional theory (DFT) calculations revealed that the SiO x ‐decoration made the surface morphology of Ni nanoparticles highly rough and step‐abundant due to the significant stabilization of low‐coordination‐number sites. The SiO x ‐decorated Ni exhibited 50 times higher catalytic activity for the dehydrogenation of methylcyclohexane to toluene than pure Ni. DFT calculations revealed that the Ni(211) step sites had a more favorable C−H activation than Ni(111) terrace sites and well reproduced the experimental apparent activation energies.