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Switching N-N Versus N-H Couplings in Nitrate Electroreduction With CuPd Surface Atomic Motifs
Keying Wu1, Wei Wu1, Siyuan Liu1
1Research Center for Carbon-Neutral Environmental & Energy Technology, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu, China.
Angewandte Chemie (International Ed. in English)
|February 11, 2026
Summary
This study reveals how atomic structures in copper-palladium (CuPd) catalysts dictate nitrate electroreduction (NO3-RR) outcomes. Ordered CuPd favors nitrogen (N2) production, while phase-segregated CuPd yields ammonia (NH3).
Area of Science:
- Electrochemistry
- Materials Science
- Catalysis
Background:
- Nitrate electroreduction reaction (NO3-RR) is crucial for mitigating nitrate pollution and synthesizing valuable chemicals like ammonia.
- Bimetallic catalysts, particularly CuPd, show promise for NO3-RR, but precise control over product selectivity remains a challenge.
- Understanding the atomic-level surface structure's influence on reaction pathways is key to designing efficient catalysts.
Purpose of the Study:
- To elucidate the structure-performance relationship in CuPd bimetallic catalysts for nitrate electroreduction.
- To investigate how ordered (o-CuPd) versus phase-segregated (p-CuPd) architectures influence reaction pathways and product selectivity.
- To provide insights for the rational design of catalysts for denitrification and ammonia electrosynthesis.
Main Methods:
- Synthesis and characterization of ordered (o-CuPd) and phase-segregated (p-CuPd) bimetallic catalysts.
- Electrochemical evaluation of catalytic performance, including current density and Faradaic efficiency for NO3-RR.
- In situ spectroscopic studies and Density Functional Theory (DFT) calculations to probe reaction intermediates and binding strengths.
Main Results:
- Ordered CuPd (o-CuPd) selectively produced dinitrogen (N2) with high current density (200 mA cm-2) and Faradaic efficiency (~95%).
- Phase-segregated CuPd (p-CuPd) efficiently produced ammonia (NH3) with comparable current density (195 mA cm-2) and Faradaic efficiency (~84%).
- DFT calculations revealed that the binding strengths of *NO and *N intermediates, influenced by surface motifs (Cu-Pd vs. Cu-Cu/Pd-Pd), dictate N-N or N-H coupling pathways.
Conclusions:
- Atomic-level surface structure, specifically the presence of Cu-Pd hetero-motifs versus homo-motifs, critically controls NO3-RR product selectivity.
- The binding strength of reaction intermediates (*NO, *N) scales linearly and plays a pivotal role in determining the final product.
- This study offers fundamental insights for designing advanced bimetallic catalysts for targeted nitrate conversion.
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