Developing highly efficient catalysts for hydrogen evolution reaction (HER) play a significant role in the large-scale application of electrochemical water splitting. Here, we develop an ultrafine ordered Pt3Co NPs supported on N-doped graphene (NG), which achieves high HER activity with a small overpotential of 13 mV at 10 mA cm–2. More importantly, at the overpotential of 20 mV, the ordered Pt3Co catalyst (Pt3Co/NG-700) indicates 19.0 and 51.8 times mass activity than that of the disordered Pt3Co catalyst (Pt3Co/NG) and commercialized Pt/C catalyst, respectively. Additionally, the Pt3Co/NG-700 electrocatalyst displays outstanding long-term stability under harsh chronopotentiometry and cycling tests in the acidic media. The theory calculations reveal that the extraordinary HER performance on Pt3Co/NG-700 electrocatalyst originates from the charge redistribution of Pt induced by Co in the structurally ordered Pt3Co intermetallic. The charge redistribution of Pt facilitates the adsorption and dissociation of H* and provides a higher electron transfer and better conductivity, resulting in high HER. Our work opens new opportunities to design noble based alloy catalysts for highly efficient HER.

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Pt-based nanoclusters toward hydrogen evolution reaction (HER) remain the most promising electrocatalysts. However, the sluggish alkaline Volmer-step kinetic and the high-cost hampered progress in developing high-performance HER catalysts. Herein, we...