Atomic Structural Evolution of Single‐Layer Pt Clusters as Efficient Electrocatalysts

Abstract The rational synthesis of single‐layer noble metal directly anchored on support materials is an elusive target to accomplish for a long time. This paper reports well‐defined single‐layer Pt (Pt‐SL) clusters anchored on ultrathin TiO 2 nanosheets—as a new frontier in electrocatalysis. The structural evolution of Pt‐SL/TiO 2 via self‐assembly of single Pt atoms (Pt‐SA) is systematically recorded. Significantly, the Pt atoms of Pt‐SL/TiO 2 possess a unique electronic configuration with PtPt covalent bonds surrounded by abundant unpaired electrons. This Pt‐SL/TiO 2 catalyst presents enhanced electrochemical performance toward diverse electrocatalytic reactions (such as the hydrogen evolution reaction and the oxygen reduction reaction) compared with Pt‐SA, multilayer Pt nanoclusters, and Pt nanoparticles, suggesting an efficient new type of catalyst that can be achieved by constructing single‐layer atomic clusters on supports.