Upcycling Nitrate Waste into Power: Designing Mo Incorporated Ni–Fe Based Phosphide Nanosheets for Electrocatalytic Green Ammonia Synthesis and Zn‐Nitrate Batteries

Abstract The electrocatalytic nitrate reduction reaction (NO 3 − RR) has emerged as a promising route for simultaneous nitrate removal and ammonia (NH 3 ) synthesis. However, achieving high NH 3 yield rates and Faradaic efficiencies (FE) under neutral pH conditions remains challenging. In this work, Mo‐incorporated FeNiP (MFNP‐x; x denotes the Mo%) electrocatalysts are synthesized via a one‐step, binder‐free electrodeposition method. Incorporation of 10% Mo into the FNP lattice significantly enhances both the NH 3 yield rate and FE by suppressing side‐product formation. The optimized MFNP‐10 catalyst achieves an exceptional NH 3 yield rate of 16271.27 µg h −1 mg cat −1 and an FE of 96.45% at −0.6 V (vs RHE) in a neutral electrolyte containing 0.5 m Na 2 SO 4 and 0.1 m KNO 3 . Computational findings assisted with Machine learning (ML) and Density functional theory (DFT) reveal that Mo incorporation synergistically enhances nitrate adsorption and introduces an alternative reduction pathway with a lower activation energy barrier. Moreover, a Zn–NO 3 − battery constructed using MFNP‐10 as cathode delivers a peak power density of 9.73 mW cm −2 , excellent stability, and an NH 3 yield of 2236.27 µg h −1 mg cat −1 with 93.85% FE. This study demonstrates a facile one‐step design strategy for developing high‐performance catalysts that couple sustainable energy storage with efficient NH 3 production.