Breaking Platinum Nanoparticles to Single-Atomic Pt-C₄ Co-catalysts for Enhanced Solar-to-Hydrogen Conversion

Effective transfer and utilization of the photogenerated electrons are a key factor for achieving highly efficient H₂ generation by photocatalytic water splitting. Apart from the activity of the co-catalyst, the interface between the co-catalyst and semiconductor is of particular importance. Guided by DFT calculations, single-atom (SA) Pt doped carbon nitride (CN) is successfully synthesized for use as the co-catalyst to the semiconducting CuS. The catalyst system (Pt1-CN@CuS) exhibits an enhanced photocatalytic performance for water splitting with a H₂ production rate of 25.4 μmol h^-1 and an apparent quantum yield (AQY) of 50.3 % under the illumination of LED-530. Solar-to-hydrogen (STH) conversion efficiency is calculated to be 0.5 % under AM 1.5 illumination. This is the very first investigation of SA as the co-catalyst, which decreases the overpotential of CN during the water splitting and lowers interfacial resistance of the catalyst/co-catalyst and co-catalyst/electrolyte.