Improved Plasmonic Hot-Electron Capture in Au Nanoparticle/Polymeric Carbon Nitride by Pt Single Atoms for Broad-Spectrum Photocatalytic H(2) Evolution

Rationally designing broad-spectrum photocatalysts to harvest whole visible-light region photons and enhance solar energy conversion is a “holy grail” for researchers, but is still a challenging issue. Herein, based on the common polymeric carbon nitride (PCN), a hybrid co-catalysts system comprising plasmonic Au nanoparticles (NPs) and atomically dispersed Pt single atoms (PtSAs) with different functions was constructed to address this challenge. For the dual co-catalysts decorated PCN (PtSAs–Au(2.5)/PCN), the PCN is photoexcited to generate electrons under UV and short-wavelength visible light, and the synergetic Au NPs and PtSAs not only accelerate charge separation and transfer though Schottky junctions and metal-support bond but also act as the co-catalysts for H(2) evolution. Furthermore, the Au NPs absorb long-wavelength visible light owing to its localized surface plasmon resonance, and the adjacent PtSAs trap the plasmonic hot-electrons for H(2) evolution via direct electron transfer effect. Consequently, the PtSAs–Au(2.5)/PCN exhibits excellent broad-spectrum photocatalytic H(2) evolution activity with the H(2) evolution rate of 8.8 mmol g(−1) h(−1) at 420 nm and 264 μmol g(−1) h(−1) at 550 nm, much higher than that of Au(2.5)/PCN and PtSAs–PCN, respectively. This work provides a new strategy to design broad-spectrum photocatalysts for energy conversion reaction. [Image: see text] SUPPLEMENTARY INFORMATION: The online version contains supplementary material available at 10.1007/s40820-023-01098-2.