A computational study of design and performance investigation of Ni-based electrocatalysts for efficient electrocatalytic hydrogen evolution reaction†

Given the current energy shortage, hydrogen energy is an attractive option as a renewable green energy source. Electrocatalytic hydrogen production is a promising and efficient method with great potential for renewable energy. However, the main limiting factor is developing low-cost and high-efficiency imprinted hydrogen evolution reaction (HER) catalysts. This study utilized theoretical calculations to address the challenge of designing Ni-based catalysts for efficient electrocatalytic HER. Firstly, Ni(111) and Ni(311) were subjected to Co doping, and the catalytic activity of Ni–Co catalysts for the electrocatalytic HER was evaluated using the ΔG_{H_ads} and E_{H2O_ads} indices. Moreover, Mo-doping modification was carried out on catalysts with more negative E_{H2O_ads} and smaller absolute values of ΔG_{H_ads} to determine the optimal catalysts for the electrocatalytic HER. Through quantum chemical calculations, the Ni(311)–2Ni–1Co-3,4Mo catalyst with optimal HER catalytic activity was determined. Additionally, the density of states (DOS) values before and after the adsorption of H* and H₂O were calculated, and the reaction pathways before and after doping were explored. The Ni(311)–2Ni–1Co-3,4Mo catalyst can dissociate H₂O and adsorb H* with higher performance, proving its excellent electrocatalytic HER catalytic performance. The findings of this study may provide theoretical guidance for the experimental development of HER catalysts.