(NiZnMg)MoN with optimized d-band center enables industrial-level hydrogen production

Abstract Developing efficient hydrogen evolution reaction (HER) electrocatalysts based on earth-abundant elements is critical for advancing sustainable energy technologies. However, existing catalysts suffer from suboptimal Gibbs free energy for hydrogen adsorption (ΔG _H*), resulting in significantly lower catalytic performance compared to platinum-based catalysts. In this study, a novel electronegativity modulation strategy was applied to enhance catalytic activity. Inspired by the d-band center (E _d) theory, Zn and Mg were introduced into the catalyst system to regulate the electronic structure. The electronegativity difference induced strong local electronic interactions, which effectively tuned the d-band center of Ni active sites and optimized ΔG _H*. As a result, the (NiZnMg)MoN catalyst exhibited outstanding HER performance with an overpotential of only 138 mV at 300 mA cm⁻², surpassing commercial Pt/C catalysts. This study provides valuable insights into designing efficient doped electrocatalysts based on d-band tuning and electronegativity engineering. The findings offer a promising strategy to overcome performance limitations in HER electrocatalysis and accelerate the practical application of alkaline hydrogen production in sustainable energy systems.