High‐Density Lewis Acid Sites in Porous Single‐Crystalline Monoliths to Enhance Propane Dehydrogenation at Reduced Temperatures

The non‐oxidative dehydrogenation of propane to propylene plays an important role in the light‐olefin chemical industry. However, the conversion and selectivity remain a fundamental challenge at low temperatures. Here we create and engineer high‐density Lewis acid sites at well‐defined surfaces in porous single‐crystalline Mo 2 N and MoN monoliths to enhance the non‐oxidative dehydrogenation of propane to propylene. The top‐layer Mo ions with unsaturated Mo‐N 1/6 and Mo‐N 1/3 coordination structures provide high‐density Lewis acid sites at the surface, leading to the effective activation of C−H bonds without the overcracking of C−C bonds during the non‐oxidative dehydrogenation of propane. We demonstrate a propane conversion of ≈11 % and a propylene selectivity of ≈95 % with porous single‐crystalline Mo 2 N and MoN monoliths at 500 °C.