Evolution of Mn‐Modified Silicalite‐1 Zeolite‐supported Nanocatalysts with the Regulated Pt–Ce Linkages for Propane Dehydrogenation

Abstract Propane dehydrogenation (PDH) is a pivotal technology for propylene production. Supported Pt catalysts for PDH are often subjected to nanoparticle agglomeration and coke deposition, thus limiting their stability and efficiency. Herein, we constructed a high‐performance Pt‐Ce catalyst consisting of CeO x with redox properties and active Pt species with the regulated electronic properties. Through the controllable impregnation, the unique structure of adjacent Pt‐CeO x sites were elaborately supported on the Mn‐modified Silicalite‐1 (Mn‐S‐1). Characterization results reveal that the generated Ce 3+ /V O species contribute to the formation of electron‐deficient Pt 0 ‐V O ‐Ce 3+ active sites via hydrogen spillover and electron transfer. Benefiting from the high dispersion of active components, appropriate acidity, redox activity of V O , and electron‐deficient Pt 0 sites, the optimal 0.5Pt0.2Ce/Mn‐S‐1 catalyst exhibits superior propane conversion of 38.23%, propylene selectivity of 88.45%, and excellent coke resistance. This study not only reveals the intrinsic correlation between active Pt and CeO x species but also provides valuable guidance for designing highly efficient catalysts.