Highly Efficient Dehydrogenation From Methylcyclohexane Over Pt Supported on Mesoporous Ni‐Al Composite Oxide With Excellent Textural and Surface Properties

ABSTRACT

Mesoporous Ni‐Al composite oxide (MNA) with excellent textural and surface properties was prepared using a facile calcination‐induced metal heteroatom doping approach and was evaluated as support of Pt‐based catalyst for methylcyclohexane dehydrogenation at a low temperature. The homogeneous incorporation of Ni atoms into the mesoporous framework of alumina and the formation of surface Ni‐O‐Al bonds benefit the generation of surface coordinated unsaturated aluminum species, which play a crucial role in highly homogenously dispersing Pt active sites in a form of single‐atom clusters. Consequently, the resultant catalyst Pt/MNA displayed significantly improved catalytic performance. For example, at 300°C, catalyst Pt/MNA demonstrated a notable catalytic activity with a maximum hydrogen evolution rate of 3057 mmol/g_Pt/min, even after a long‐time reaction up to 100 h or regeneration, which is inspiringly superior to the state‐of‐the‐art supported Pt‐based catalysts. The obviously boosted catalytic reactivity of catalyst Pt/MNA can be attributed to the excellent structural and textural properties, the remarkably raised Pt utilization efficiency, and the synergic catalytic effect derived from the interface electron transfer from support MNA to metallic Pt active sites. Our results provided a rational design strategy for the development of promising Pt‐based catalyst for methylcyclohexane dehydrogenation, which is vital in the utilization of methylcyclohexane–toluene system for hydrogen storage.