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 nanosheets-as a new frontier in electrocatalysis. The structural evolution of Pt-SL/TiO via self-assembly of single Pt atoms (Pt-SA) is systematically recorded. Significantly, the Pt atoms of Pt-SL/TiO possess a unique electronic configuration with PtPt covalent bonds surrounded by abundant unpaired electrons. This Pt-SL/TiO 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.
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