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

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 CeOx and Pt clusters within silicalite-1 (S-1) zeolite. Zeolite confinement stabilizes both Pt and CeOx species under reducing dehydrogenation conditions, while the dynamic and reversible formation of strong Pt-CeOx interactions facilitates the reversible redispersion of Pt species during oxidative regeneration. Notably, the Pt-4CeOx@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 CeOx to dynamically capture mobile PtOx 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.