Pt Atoms/Clusters on Ni-phytate-sensitized Carbon Nitride for Enhanced NIR-light-driven Overall Water Splitting beyond 800 nm.

Near-infrared (NIR) light-driven overall water splitting beyond 800 nm remains a high-priority target yet great challenge. Here we report that efficient utilization of photogenerated electrons in a photosensitized system prepared by site-selective photodeposition of platinum single atoms/clusters (Pt-SACs) on Ni-phytate (PA-Ni)-sensitized polymeric carbon nitride (PCN). The optimal catalyst presents simultaneous hydrogen (H 2 ) and oxygen (O 2 ) evolution with an H 2 evolution amount of 1.4 μmol at λ>800 nm for 24 hours, which its activity was approximately 140 times higher than that of a system without Pt-SAC modification (PA-Ni 1.1 @PCN). This work represents the first NIR-light responsive photosensitized system for overall water splitting, and may open an avenue for precisely manipulating cocatalyst positions at the atomic level to improve NIR-light-driven overall water splitting via photosensitization.