Construction of Electron-Enriched Pt^δ+ with Reactive Oxygen Species for Enhanced Propane Catalytic Combustion

The complete catalytic oxidation of propane (C₃H₈) at low temperatures remains challenging due to the competitive adsorption between the oxidation of the O₂ and C₃H₈ molecules. In this study, we propose an innovative approach to enhance C₃H₈ oxidation by strategically designing active Pt^δ+ sites with modulated electronic structures on F-doped TiO₂-supported Pt catalyst (Pt/F-TiO₂), which exhibits 50 and 90% of propane conversion at 200 and 320 °C. Our mechanistic study reveals that the electron coupling between Pt 5d and F 2p alters the d orbital electron property, which leads to generation of abundant efficient electron-enriched Pt^δ+ species. These new Pt^δ+ sites facilitate the adsorption of C₃H₈ and promote the activation of chemisorbed O₂ into superoxide species, in the form of bridge Pt-(O-O)_ad-Ti, which synergistically facilitates the methyl C-H cleavage in C₃H₈. This study presents the strategy for electronic structure engineering of active sites in Pt-based catalysts, paving the way for the development of high-performance catalysts for propane oxidation.