Directional CO spillover promotes C–N coupling for highly selective electrocatalytic urea production

Abstract

Electrocatalytic co-reduction of nitrate (NO3/NO2) and CO2 to urea offers a sustainable pathway for simultaneous wastewater remediation and fertilizer synthesis, but its efficiency is plagued by sluggish C–N coupling kinetics and a mismatched reaction rate of CO2 and NO3 reduction. Herein, we design a tandem electrode composed of zinc nanoparticles on copper nanowires that spatially decouples NO3 activation and *CO generation, enabling directional intermediate spillover for enhanced C–N coupling. The minimized work function difference between Zn and Cu facilitates spontaneous *CO migration from Zn (CO2 → *CO) to Cu (NO3 → *NH2), achieving a faradaic efficiency of ∼99% and a urea production rate of 191.2 μg h−1 cm−2 at ultralow overpotential. In situ Raman and density functional theory calculations confirm that this architecture circumvents kinetic limitations of single-site catalysts by segregating and synchronizing key intermediates. Our work establishes a paradigm for precision control in multi-reactant electrocatalysis through spatially modulated tandem active sites.

Graphical abstract: Directional CO spillover promotes C–N coupling for highly selective electrocatalytic urea production

Supplementary files

Article information

Article type
Paper
Submitted
17 Jul 2025
Accepted
06 Oct 2025
First published
13 Oct 2025

Green Chem., 2025, Advance Article

Directional CO spillover promotes C–N coupling for highly selective electrocatalytic urea production

S. Chang, J. Gao, Y. Xuan and K. Wang, Green Chem., 2025, Advance Article , DOI: 10.1039/D5GC03681J

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