Enhancing Photocatalytic Propane Dehydrogenation via Electronic Structure Modulation of Platinum Sites Over Platinum‐Based Alloys

ABSTRACT Photocatalytic propane dehydrogenation (PDH) offers a promising route for propylene production under mild conditions despite the unsatisfactory propylene yield at present. Herein, we have introduced several second metals into Pt/ZnO catalyst to modulate the electronic structure of Pt by forming PtM alloys. Among all these catalysts, PtPb alloys/ZnO catalyst (PtPb/ZnO) exhibits the optimum photocatalytic PDH activity. Both experiments and density functional theory calculations reveals that PtPb alloys significantly increases the electron density of Pt, weakening the interaction between Pt and propylene. This facilitates the desorption of the produced propylene during photocatalytic PDH, thus helping to release Pt active sites for reactant conversion. A 3.6‐fold increase on propylene yield of photocatalytic PDH has been achieved over PtPb/ZnO with a propylene production rate of 5.4 mmol g −1 h −1 . Our findings highlight the critical relationship between the electronic structure of Pt active sites and performance, marking product desorption modulation an effective strategy to boost photocatalytic PDH.