Atomically dispersed Pt species anchored on Al3+-doped SrTiO3 for photocatalytic overall water splitting
Single-atom co-catalysts on semiconductor substrates offer a cost-efficient route to enhance photocatalytic performance with minimal precious metal loading. However, precise tuning of local coordination environments and construction of efficient single-atom co-catalysts remain challenging for overall water splitting. Here, we employ an icing-assisted photochemical reduction strategy to anchor atomically dispersed Pt species as hydrogen evolution co-catalysts on Al3+-doped SrTiO3 (Pt SA-STO). The optimized Pt SA-STO exhibits remarkable activity, with hydrogen and oxygen evolution rates of 13.62 and 6.71 mmol h−1 g−1, respectively, and a turnover frequency (TOF) of 2114.5 h−1. We pioneer the use of nuclear magnetic resonance (NMR) spectroscopy to quantitatively track the temporal evolution of Pt4+ to Pt2+ under continuous irradiation during the icing-assisted photoreduction. Advanced characterizations and theoretical calculations confirm that single-atom Pt co-catalysts facilitate directional transfer and extraction of photogenerated charge carriers, effectively suppressing surface recombination. This work provides insights into designing novel single-atom co-catalysts by deepening understanding of electronic configurations and active sites in photocatalytic overall water splitting.