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Electrochemical reduction of contaminated nitrate to ammonia (NRA) opens a new window for mass production of ammonia and the alleviation of energy crises and environmental pollution. However, fabricating effective catalysts for the NRA still faces significant challenges. Herein, a highly-efficient NRA catalyst, FeP 4 /Ni 2 P, was successfully constructed. The strong electron coupling at heterointerfaces of FeP 4 /Ni 2 P promoted the generation of abundant active hydrogen *H, inhibited the competition of the HER, accelerated the hydrogenation of the NRA. Benefiting from these, the catalyst displays good NRA catalytic activity in the neutral electrolyte, with the NH 3 FE of 97.83 ± 0.091 %, NH 3 selectivity of 98.67 ± 0.50 %, NH 3 yield rate of 0.262 ± 0.01 mmol·h -1 ·cm -2 , and NO 3 - conversion rate of 93.02 ± 0.14 %. The DFT theoretical calculations demonstrated that the FeP 4 /Ni 2 P heterointerfaces played a critical role in shearing the H-OH bonds of water, resulting in generating more active hydrogen as a key NRA hydrogenation source, and hindering the *H dimerization to form H 2 , enhancing the NH 3 selectivity. This work has a certain reference value for designing excellent catalysts for the NRA., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Inc. All rights reserved.)