Abstract
Photocatalytic reforming (PR) of polyester waste, fueled by renewable sources like solar energy, offers a sustainable method for producing clean H(2) and valuable by-products under mild conditions. The design of high-performance photocatalyst plays a pivotal role in determining the efficacy of an alkaline polyester PR system, influencing H(2) generation activity and selectivity. Here, ultrathin porous carbon nitride nanosheets (UP-CN) loaded with Pt nanoclusters (Pt NCs, average diameter of 1.7 nm) with uniform Pt NCs distribution are introduced. The resulting Pt NCs/UP-CN catalyst can accelerate charge and mass transfer while providing additional active sites, achieving superior H(2) generation rates of 11.69 mmol g(cat) (-1) h(-1) and 2923 mmol g(Pt) (-1) h(-1) under AM 1.5 light, which nine times higher than that of Pt nanoparticles-bulk graphitic carbon nitride composite (1.29 mmol g(cat) (-1) h(-1) and 258 mmol g(Pt) (-1) h(-1)) as counterpart. This performance also surpasses that of previously reported carbon nitride-based and TiO(2)-based photocatalysts. Moreover, the density functional theory calculations reveal a significant reduction in the energy barrier for the water dissociation step (H(2)O + * → *H + OH) at the interface between UP-CN and anchored Pt NCs, showcasing the synergistic effect between Pt NCs and UP-CN. This catalytic system also exhibits universality across various polyester plastics.