Built‐In Self‐Regeneration of Platinum Catalysis in Propane Dehydrogenation with Rare‐Earth‐Modified Zeolites

ABSTRACT Platinum‐based zeolite catalysts are among the most effective systems for propane dehydrogenation (PDH), yet their industrial deployment is limited by their poor regenerability under harsh redox cycling. Here, we report a ligand‐protected strategy to simultaneously encapsulate subnanometric CeO x and Pt clusters within silicalite‐1 (S‐1) zeolite. Zeolite confinement stabilizes both Pt and CeO x species under reducing dehydrogenation conditions, while the dynamic and reversible formation of strong Pt–CeO x interactions facilitates the reversible redispersion of Pt species during oxidative regeneration. Notably, the Pt‐4CeO x @S‐1 catalyst remains fully regenerable after 9 consecutive redox cycles and sustained operation over 5000 min at 600°C. Even after steam treatment at 600°C, the catalyst fully recovers its activity through simple calcination–reduction, demonstrating outstanding structural durability under industrially relevant conditions. Integrated theoretical and experimental evidence shows that confinement within the zeolite framework allows CeO x to dynamically capture mobile PtO x via Pt–O‒Ce bond formation, facilitating atomic‐scale Pt redispersion under oxidative conditions. This work offers a generalizable strategy for constructing redox‐adaptive catalyst architectures with built‐in self‐regeneration, advancing the design of robust zeolite‐based catalysts for high‐temperature and cyclic catalytic processes.