Breaking Barriers: Synergistic Interactions Between Pt Single Atoms and Nitrogen‐Rich g‐C3N4 for Maximized Photocatalytic Hydrogen Production

Abstract Designing an active catalyst and an in situ route for the decoration of single atoms (SA) on graphitic carbon nitride (C 3 N 4 ) toward efficient photocatalytic H 2 evolution reaction has been a wide area of focus. However, ultralow loading of SAs and miniaturizing of the catalyst with excess nitrogen for maximized photocatalytic H 2 production from water remains challenging. Herein, a simple novel method is demonstrated to fasten ultralow concentration of Pt atom (0.08 wt.%) on template‐based N‐rich C 3 N 4 (C 3 N 4.6 ) via thermal polymerization and acid leaching method to get a visible light irradiation‐based H 2 production rate of 64100 µmol g −1 h −1 , with an apparent quantum yield of 25.3%, and long‐term stability. The synthesis process involves initially attaching platinum complex to SBA‐15, thermal polymerization of dicyandiamide, and the formation of Pt SAs anchored on the surface of C 3 N 4.6 . Pt SAs are found to coordinate and interact with the N‐rich sites and alter the electronic structure of the C 3 N 4.6 . The atomically dispersed Pt species not only act as a sink for photoexcited electrons but also work as reduction sites to facilitate the faster water reduction kinetics on the surface than Pt NP decorated C 3 N 4 , highlighting the potential of ultralow‐loading Pt‐SACs in promoting sustainable H 2 production.