Cooperation of PtO 2 and Adjacent Pt 1 on In 2 O 3 Photocatalysts for Unity‐Selective Propane Dehydrogenation

Solar‐driven direct propane dehydrogenation (PDH) represents a promising strategy to overcome the high‐temperature demands and selectivity limitations of conventional thermocatalysis, yet the identification of effective photoactive phases remains challenging. Herein, we demonstrate that photoactivated PtO 2 enables regenerable and highly selective PDH over a PtO 2 /Pt 1 ‐In 2 O 3 catalyst under mild conditions. Under simulated sunlight without external heating, the catalyst achieves a propylene formation rate of 1322.35 µmol g −1 h −1 with unity selectivity, while remaining inactive under comparable thermocatalytic conditions. In situ spectroscopic analyses combined with density functional theory calculations reveal a photoactivated dual‐site mechanism, in which PtO 2 nanoparticles function as oxidation centers for hole‐driven C─H bond activation, whereas neighboring interfacial Pt single atoms act as electron‐accepting sites to promote H 2 evolution, enabling efficient spatial separation and utilization of photogenerated charge carriers. Catalyst deactivation arises from partial reduction of PtO 2 , which can be exactly regenerated via a facile oxidative annealing process in air, affording excellent reusability. These findings identify photoactivated PtO 2 as a distinct active phase for selective PDH and provide a design principle for solar‐driven alkane valorization.