“…have gained considerable limelight for their promising performance toward OER, their high cost and scarcity have limited their usage on an industrial scale. , The earth-abundant base metals such as Co, Ni, Mn, Fe, etc., cover the current interest in developing economic and productive electrocatalysts for OER. − Among these metals, Ni-based materials have gained peculiar attention for their high water oxidation efficiency and low overpotentials. , In fact, the hydroxides and oxides based on Ni metal are one of the best-studied candidates for OER, owing to their high reaction rates and low overpotential values . Meanwhile, for these nickel oxides/hydroxides, the difficulty in accurately identifying and describing the reactive surface structure and the active site has caused a large variation in the literature values for OER onset potential, overpotential, and reaction kinetics. − Recent approaches, such as computational studies, have been successfully employed to understand atomic-level models for describing electrochemical OER reaction kinetics and mechanisms. ,, Meanwhile, the studies employing nickel-based oxides/hydroxide catalysts often require an approximation to the model systems during the computational studies, as they lack a well-defined catalytic structure, and the activity is dependent on the molecular packing. − However, it is important to describe the realistic working catalysts to facilitate the structure modifications for improving catalytic performances and identifying the structure–activity relationships …”