What question did this study set out to answer?

The aim is to understand how surface structures of CuPd catalysts influence nitrate reduction pathways and product formation.

February 12, 2026

Switching N‐N Versus N‐H Couplings in Nitrate Electroreduction With CuPd Surface Atomic Motifs

Key Points

The aim is to understand how surface structures of CuPd catalysts influence nitrate reduction pathways and product formation.
Utilized ordered (o‐CuPd) and phase‐segregated (p‐CuPd) bimetallic catalyst architectures.
Conducted in situ studies and density functional theory (DFT) calculations to analyze intermediate binding.
Measured current densities and Faradaic efficiencies for nitrogen and ammonia production.
o‐CuPd achieved selective N2 production with a current density of 200 mA cm−2 and ∼95% Faradaic efficiency.
p‐CuPd enabled NH3 formation with 195 mA cm−2 and ∼84% Faradaic efficiency.
Binding strengths of *NO intermediates and their relationship with *N were crucial in determining product pathways.

Abstract

ABSTRACT Nitrate electroreduction reaction (NO 3 − RR) offers a promising solution to address excessive nitrate emissions by converting them into either environmentally benign dinitrogen or useful ammonia. Bimetallic catalysts, such as CuPd, have been recognized to be active for NO 3 − RR. However, the product discrepancies over bimetallic catalysts hinder further rational construction, largely owing to the poor understanding of how atomic‐level surface structures precisely control post‐NO reduction pathways via crucial intermediates binding. Herein, we take CuPd as model bimetallic catalysts with ordered (o‐CuPd) and phase‐segregated (p‐CuPd) architectures, featuring Cu‐Pd hetero‐motifs and Cu‐Cu/Pd‐Pd homo‐motifs on the surface, respectively, to elucidate the structure‐performance relationship. The o‐CuPd enabled selective N 2 production with a current density up to 200 mA cm −2 and Faradaic efficiency of ∼95%, whereas the p‐CuPd achieved NH 3 formation with 195 mA cm −2 and ∼84% FE. Multiple in situ studies and DFT calculations disclosed that the binding strength of *NO intermediates scales linearly with that of *N, and their adsorption strengths over Cu‐Pd and Cu‐Cu or Pd‐Pd motifs play a crucial role in determining the post‐NO reduction pathways towards either N‐N or N‐H couplings, resulting in distinct final products. This work provides new insights for the rational construction of bimetallic catalysts for denitrification and ammonia electrosynthesis.

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