A high-density nickel–cobalt alloy embedded in nitrogen-doped carbon nanosheets for the hydrogen evolution reaction

Abstract

The development of novel non-noble electrocatalysts is critical for an efficient electrochemical hydrogen evolution reaction (HER). In this study, high-density nickel–cobalt alloy nanoparticles embedded in the bent nitrogen-doped carbon nanosheets are prepared as a high-performance catalyst. The optimized Ni₇Co₃/NC-500 catalyst displays quite a low overpotential of 90 mV at a current density of 10 mA cm⁻², and a small Tafel slope of 64 mV dec⁻¹ in alkaline medium, and even performs better than commercial 20% Pt/C at a high current density (η₁₅₀ = 233 mV for Ni₇Co₃/NC-500 and η₁₅₀ = 267 mV for 20% Pt/C). Specifically, the high-density nickel–cobalt alloy (with an average size of 6.2 nm and a distance of <3.0 nm) embedded in the bent carbon nanosheets provides plentiful active sites. Furthermore, in situ visualization of the produced hydrogen bubbles shows that the small size of hydrogen bubbles (d = 0.2 mm for Ni₇Co₃/NC-500 vs. d = 0.8 mm for 20% Pt/C) resulting from the small water contact angle and the bent nanosheet structure would inhibit the aggregation of H₂ bubbles on the surface to facilitate efficient mass diffusion. Density functional theory calculations reveal that the formation of the nickel–cobalt alloy can effectively lower water dissociation energy barriers and optimize hydrogen adsorption Gibbs free energy, manifesting a high HER activity.