Optimizing Nickel‐Based Electrocatalysts for Hydrogen and Oxygen Evolution: Electronic and Geometric Perspectives

Abstract Electrochemical water splitting is a promising approach for sustainable hydrogen production, yet the development of cost‐effective and efficient electrocatalysts remains a critical challenge. Nickel‐based materials have emerged as viable alternatives to noble metal catalysts due to their abundance, tunable electronic structure, and comparable catalytic activity. This review systematically summarizes recent advances in nickel‐based electrocatalysts for hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and overall water splitting (OWS). Based on the catalytic mechanism of the above reactions, electronic structure modulation from a thermodynamic adsorption/desorption optimization perspective and geometric structure optimization from a diffusion kinetic improvement perspective are proposed for a high‐performance Ni‐based electrocatalyst. Key strategies include morphology engineering, alloying, heteroatom doping, phase engineering, and heterostructure construction, which optimize intermediate adsorption/desorption, charge transfer, and mass transport kinetics. Despite significant progress, challenges persist in achieving industrial‐scale current densities (>500 mA cm −2 ) and long‐term stability. Future efforts should focus on multiscale design, high‐current‐density testing, and mechanistic studies to bridge the gap between laboratory research and practical applications. This review provides valuable insights for designing highly efficient Ni‐based electrocatalysts toward scalable green hydrogen production.