Alkaline hydrogen evolution reaction (HER) represents a promising means to store intermittent renewable energy into clean energy. Unfortunately, the sluggish H2O dissociation and difficult *H adsorption-desorption are prominent obstacles to the development of alkaline HER. Herein, we developed a cooperative strategy via nanoneedle inducing local electric field and atomic doping causing electron localization for alkaline HER based on the preparation of Cu doped CoS2 nanoneedles (Cu-CoS2 NNs). Finite element method simulations and density functional theorycalculations demonstrate the local electric field accelerates H2O dissociation and electron localization facilitates *H adsorption, respectively. In situ attenuated total reflection infrared spectroscopy and electro-response measurement experimentally reveal the superior ability to H2O dissociation and *H adsorption for Cu-CoS2 NNs. As a result, the Cu-CoS2 NNs exhibit an ultralow overpotential of 64 mV at –10 mA cm−2 and long-term stability over 100 h at –100 mA cm−2 during alkaline HER, which outperforms most electrocatalysts in recently published works.
