▎ 摘　　要

Developing high-performance Pt-based alloy catalysts with strong metal-support interaction is considered an effective strategy to optimise the intrinsic activity and stability of catalysts and has received extensive attention, but still challenging. Herein, Pt3Ni alloy nanoparticles coupled with three-dimensional N-doped graphene (Pt3Ni/3DNG) are prepared and used for enhancing the alkaline hydrogen evolution reaction (HER). It is found that the Pt3Ni/3DNG catalyst generates a tensile strain and give rise to a ligand effect on the surface of the active sites, which efficiently boost water dissociation and optimise H* desorption, thereby accelerating the alkaline HER kinetics. As a result, the Pt3Ni/3DNG catalyst exhibits an exceptional alkaline HER activity with a mass activity 14 times that of commercial 40 wt.% Pt/C at 70 mV and a high stability (no decay is observed after 10,000 cycles). This work demonstrates the function of quaternary-N and pyridinic-N in the HER, and provides a novel design for Pt-based alloy catalysts with high alkaline HER performance.