Gas‐Phase Activation‐Driven Interface Modulation of Pt‐Based Catalysts for Selective and Stable Propane Dehydrogenation

Abstract Propane dehydrogenation (PDH) is a key industrial process for on‐demand propylene production, yet catalyst deactivation due to coke formation and metal sintering remains a critical challenge. In this work, we introduce a novel activation strategy that simultaneously modulates metal‐support interactions (MSI) and acidity in Pt‐based catalysts through a sequential CH 4 /H 2 followed by pure H₂ pretreatment. This tailored approach enhances the electronic density of Pt nanoparticles and the distribution of acid sites, rationally tuning MSI to achieve a synergistic enhancement in activity, selectivity, and durability. As a result, the optimized catalyst exhibits exceptional PDH activity, achieving a 59.7 mmol·g cat ⁻ 1 ·h⁻ 1 propylene formation rate with 94.1% selectivity and an extended operational lifetime. The findings provide additional understanding of how activation atmospheres influence catalyst structure and reactivity, contributing to the ongoing development of efficient and stable PDH catalysts.