Highly Stable Propane Dehydrogenation on a Self‐supporting Single‐component Zn2SiO4 Catalyst

Current industrial propane dehydrogenation (PDH) processes predominantly use either toxic Cr‐based or expensive Pt‐based catalysts, necessitating urgent exploration for alternatives. Herein, we present Zn2SiO4, an easily prepared, cost‐effective material, as a highly efficient and stable catalyst for PDH. Uniquely, Zn2SiO4 nanocrystals do not require dispersion on support materials, commonly needed for catalytic active oxide clusters, but function as a self‐supporting catalyst instead. During the reaction's induction period, surface Zn species on the Zn2SiO4 crystal reduce to coordinately unsaturated ZnOx single sites, serving as highly active catalytic centers. The Zn2SiO4 catalyst demonstrates a stable performance over 200 hours of PDH operation at 550 °C. We further find that introducing a minuscule amount of CO2 into the propane feed significantly extends the catalyst lifespan to over 2000 hours. This enhancement arises from the special role of CO2 in facilitating the removal of strongly adsorbed H*, preventing the complete reduction of ZnOx. After prolonged reaction, the activity of Zn2SiO4 can be fully restored by etching the surface layer to expose fresh Zn species, available throughout the crystals. The combination of CO2 introduction and catalytic site regeneration strategies is expected to enable a year‐long PDH operation using a single batch of Zn2SiO4 catalyst.