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This research focuses on improving ammonia synthesis from nitrate reduction using a novel tandem catalyst.

July 10, 2026Small0 citations

Hierarchical Electronic Structure Modulation of Cu‐Co Dual‐Site and CNT Tandem Interface Enables Highly Efficient Electrocatalytic Ammonia Synthesis

ZSZhi SongState Ethnic Affairs Commission DHDongxu HanState Ethnic Affairs Commission BLBoxia LiuNorth Minzu University

Key Points

This research focuses on improving ammonia synthesis from nitrate reduction using a novel tandem catalyst.
Designed a tandem catalyst Cu‐Co‐O/CNT-2 using carbon nanotubes as support.
Characterized catalyst performance under neutral electrolyte conditions.
Utilized DFT calculations and FTIR to analyze reaction pathways and electronic structure.
Achieved an ammonia yield of 5.088 mg h −1 cm −2 at −0.9 V vs RHE with a Faradaic efficiency of 81.83%.
In situ FTIR analysis confirmed the NHO pathway with the capture of the * NH 2 OH intermediate.
DFT calculations showed effective adsorption of * NO x on the Cu‐Co‐O sites, enhancing overall catalytic efficiency.

Abstract

ABSTRACT Electrocatalytic reduction of nitrate to ammonia (NO 3 RR) is a highly efficient dual strategy that can both reduce NO 3 − pollution and achieve sustainable NH 3 production. To overcome the low efficiency bottleneck under neutral electrolyte conditions, this study designed a tandem catalyst Cu‐Co‐O/CNT‐2 based on carbon nanotubes (CNT). By anchoring the Cu‐Co dual sites on the CNT support, the electronic structure and reaction pathway were optimized. At −0.9 V vs RHE, the Cu‐Co‐O/CNT‐2 catalyst exhibited an ammonia yield of 5.088 mg h −1 cm −2 and a Faradaic efficiency of 81.83%, significantly improving the NO 3 RR performance. In situ FTIR characterization revealed the dominant NHO pathway and successfully captured the * NH 2 OH intermediate. DFT calculations and in situ EPR analysis further indicate that the Cu‐Co‐O active sites preferentially adsorb * NO x , while CNT effectively lowers the reaction energy barrier and enhances the multi‐electron conversion efficiency by promoting the upward shift of the d‐band center (−1.837 eV), thus driving the deoxygenation and stepwise hydrogenation of NO 3 − to NH 3 . In summary, this study provides theoretical support for the design of efficient tandem catalytic systems and offers new insights into ammonia generation and resource conversion in the NO 3 RR reaction.

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