Highly Stable Propane Dehydrogenation on a Self‐Supporting Single‐Component Zn₂SiO₄ Catalyst

Abstract 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 Zn 2 SiO 4 , an easily prepared, cost‐effective material, as a highly efficient and stable catalyst for PDH. Uniquely, Zn 2 SiO 4 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 Zn 2 SiO 4 crystal reduce to coordinately unsaturated ZnO x single sites, serving as highly active catalytic centers. The Zn 2 SiO 4 catalyst demonstrates a stable performance over 200 hours of PDH operation at 550 °C. We further find that introducing a minuscule amount of CO 2 into the propane feed significantly extends the catalyst lifespan to over 2000 hours. This enhancement arises from the special role of CO 2 in facilitating the removal of strongly adsorbed H*, preventing the complete reduction of ZnO x . After prolonged reaction, the activity of Zn 2 SiO 4 can be fully restored by etching the surface layer to expose fresh Zn species, available throughout the crystals. The combination of CO 2 introduction and catalytic site regeneration strategies is expected to enable a year‐long PDH operation using a single batch of Zn 2 SiO 4 catalyst.