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

Designing an active catalyst and an in situ route for the decoration of single atoms (SA) on graphitic carbon nitride (C₃N₄) toward efficient photocatalytic H₂ 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 H₂ 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 C₃N₄ (C₃N_4.6) via thermal polymerization and acid leaching method to get a visible light irradiation-based H₂ 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 C₃N_4.6. Pt SAs are found to coordinate and interact with the N-rich sites and alter the electronic structure of the C₃N_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 C₃N₄, highlighting the potential of ultralow-loading Pt-SACs in promoting sustainable H₂ production.