The employment of single atoms (SAs), especially Pt SAs, as co-catalysts in photocatalytic H2 generation has gained significant attention due to their exceptional efficiency. However, a major challenge in their application is the light-induced agglomeration of these SAs into less active nanosized particles under photocatalytic conditions. This study addresses the stability and reactivity of Pt SAs on TiO2 surfaces by investigating various post-deposition annealing treatments in air, Ar, and Ar-H2 environments at different temperatures. It is described that annealing in an Ar-H2 atmosphere optimally stabilizes SA configurations, forming stable 2D rafts of assembled SAs ≈0.5-1 nm in diameter. These rafts not only resist light-induced agglomeration but also exhibit significantly enhanced H2 production efficiency. The findings reveal a promising approach to maintaining the high reactivity of Pt SAs while overcoming the critical challenge of their stability under photocatalytic conditions.

Department of Materials Science and Engineering Chair for Surface Science and Corrosion Friedrich Alexander Universität Erlangen Nürnberg Martensstraße 7 91058 Erlangen Germany

Institute of Catalysis Research and Technology and Institute for Chemical Technology and Polymer Chemistry Karlsruhe Institute of Technology 76131 Karlsruhe Germany

Institute of Catalysis Research and Technology Karlsruhe Institute of Technology 76344 Eggenstein Leopoldshafen Germany

Regional Centre of Advanced Technologies and Materials Šlechtitelů 27 Olomouc 78371 Czech Republic

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