Breaking Barriers: Synergistic Interactions Between Pt Single Atoms and Nitrogen-Rich g-CN 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 (CN) toward efficient photocatalytic H 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 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 CN (CN) via thermal polymerization and acid leaching method to get a visible light irradiation-based H production rate of 64100 µmol g h, 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 CN. Pt SAs are found to coordinate and interact with the N-rich sites and alter the electronic structure of the CN. 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 CN, highlighting the potential of ultralow-loading Pt-SACs in promoting sustainable H production.