Stable Cobalt–Zeolite Propane‐Dehydrogenation Catalysts Enabled by Reaction‐Driven Reconstruction

Abstract Cobalt‐based catalysts have emerged as promising substitutes for Pt‐ and Cr‐based propane dehydrogenation (PDH) catalysts. However, controlling the distribution of Co species and achieving stable active centers remains challenging. Here, we report that reaction‐driven reconstruction of metallic cobalt (Co 0 ) species within pure silica MFI zeolite (S‐1) into CoO x clusters within silanol nests during PDH yields efficient and durable performance. Atomically dispersed CoO x clusters exhibit exceptional durability and high propylene space‐time yield (STY), maintaining an ultrahigh propylene STY of 17.2 mmol C3H6 g cat −1 h −1 for over 260 h under industrially relevant conditions, surpassing previous cobalt‐based PDH catalysts. Moreover, the catalyst operates stably at 520 °C for 170 h with near‐equilibrium propane conversions. Comprehensive characterizations indicate the dynamic evolution process from the silanol nests effectively capturing and stabilizing Co 0 species within S‐1 zeolite, thereby promoting the dynamic formation of CoO x clusters during the PDH process. We also demonstrate that stable Co─O active centers formed by this unique anchoring strategy improve catalyst stability by suppressing coke formation and promoting efficient propane dehydrogenation.