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September 10, 2025Open Access

Modulating Surface‐Active Hydrogen for Facilitating Nitrate‐to‐Ammonia Electroreduction on Layered Double Hydroxides Nanosheets

BLBin LiuCentral South University YWYuan WangTianjin University of Science and Technology HWHai‐Hu WenCollaborative Innovation Center of Advanced Microstructures

Key Points

A large ammonia yield of 1.64 mmol h−1 cm−2 achieved, significantly improving the efficiency of nitrate reduction.
With a Faradaic efficiency of 94.8% across 15 cycles, NiCuFe-LDHs demonstrate stability and effectiveness in the nitrite reduction process.
The method involves theoretical analysis of the nitrate reduction pathway and highlights the role of copper and nickel sites in enhancing activity.
This approach may enable efficient removal of nitrate pollutants while producing ammonia, representing a sustainable alternative to traditional methods.

Abstract

Abstract Electrocatalytic nitrate (NO 3 − ) reduction reaction (NitRR) to valuable ammonia (NH 3 ) presents a promising alternative strategy to the conventional Haber‐Bosch process, yet suffers from low Faradaic efficiency (FE) and limited NH 3 yield due to the sluggish multi‐electron/proton transfer steps involved. Here, NiCuFe‐layered double hydroxides (NiCuFe‐LDHs) nanosheets with abundant metal Ni and Cu sites are synthesized for facilitating NO 3 − ‐to‐NH 3 electroreduction with a large NH 3 yield of 1.64 mmol h −1 cm −2 , NH 3 FE of 94.8% and high stability for 15 cycles. Computational and theoretical analysis reveals the NitRR pathway and elucidates that the Cu and Ni sites act as the primary center for NO 3 − adsorption and activation. Meanwhile, the Ni site effectively modulates the adsorption and dissociation of H 2 O to provide sufficient H * , thus enhancing the NitRR activity of NiCuFe‐LDHs nanosheets. Consequently, the Zn‐NO 3 − battery utilizing NiCuFe‐LDHs nanosheets as the cathode delivers a high FE of 85.8%, a large NH 3 yield of 1.63 mmol h −1 cm −2 , and a remarkable power density of 12.4 mW cm −2 , outperforming most previous reports, which enable the simultaneous NO 3 − pollutants removal, NH 3 production, and electricity output. This work offers a promising strategy for designing and synthesizing efficient electrocatalysts for NO 3 − removal and value‐added NH 3 production.

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