Ammonia (NH3) plays an irreplaceable role in human life as a promising energy carrier and indispensable chemical raw material. Nitrate electroreduction to ammonium (NRA) not only removes nitrate pollutants, but also can be used for efficient NH3 production under ambient conditions. However, achieving high efficiency and selectivity of electrocatalysts is still a great challenge. Herein, a complex Cu2(NO3)4(BMMB)·H2O with a bicopper core is assembled by Cu(NO3)2·3H2O and

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... nzimidazolyl]methyl}benzene (BMMB) for NRA under alkaline conditions. The optimal sample showed excellent nitrate reduction performance with the NO3− conversion rate of 70%, Faradaic efficiency of up to 90%, and NH3 selectivity of more than 95%. The high-catalytic activity is mainly due to the ingeniously designed copper cores with strong affinity for NO3−, which accelerates the transferring rate of adsorbed nitrate on the Cu surface and increases the efficiency of rate-determining step (NO3− → NO2−) in the whole catalytic process. Therefore, the transformation of surface-exposed nitrate can be rapidly catalyzed by the Cu active sites, facilitating the conversion efficiency of nitrate.