Electrocatalytic reduction of nitrate has merged as one of the promising sustainable approach to remove the excess nitrate in wasterwater. Electrocatalysis enables the conversion of pollutants into valuable chemicals using clean energy. Traditionally, catalyst development relies on trial-and-error methods, but a rational design strategy necessitates a deeper understanding of the nitrate reduction process. Currently, surface-specific mechanistic insights are largely derived from theoretical models, and there is no direct experimental evidence at the molecular level.