Oxy-reductive C-N bond formation via pulsed electrolysis

Yuxuan Zhang, Hasan Al-Mahayni, Pedro M. Aguiar, Daniel Chartrand, Morgan McKee, Mehdi Shamekhi, Ali Seifitokaldani () and Nikolay Kornienko ()
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Yuxuan Zhang: Université de Montréal
Hasan Al-Mahayni: McGill University
Pedro M. Aguiar: Université de Montréal
Daniel Chartrand: Université de Montréal
Morgan McKee: Université de Montréal
Mehdi Shamekhi: Concordia University
Ali Seifitokaldani: McGill University
Nikolay Kornienko: Université de Montréal

Nature Communications, 2025, vol. 16, issue 1, 1-9

Abstract: Abstract Co-electrolysis of CO2 with simple N-species is an appealing route to sustainable fabrication of C-N bond containing products. A prominent challenge in this direction is to promote the C-N coupling step in place of the established CO2 reduction pathways. This can be particularly difficult when relying on solution-based species (e.g., NH3) to intercept intermediates that are continually being reduced on heterogeneous catalyst surfaces. In light of this, we introduce oxy-reductive pulsed electrocatalysis as a tool for C-N bond formation. The reaction routes opened through this method involve both partial reduction and partial oxidation of separate reactants on the same catalyst surface in parallel to co-adsorb their activated intermediates proximal to one another. Using CO2 and NH3 as model reactants, the end result is an enhancement of selectivity and formation rates for C-N bond containing products (urea, formamide, acetamide, methylamine) by factors of 3-20 as compared to static electrolysis in otherwise identical conditions. An array of operando measurements is carried out to pinpoint the key factors behind this performance enhancement. Finally, the oxy-reductive coupling strategy is extended to additional carbon and nitrogen reactants and is further applied to C-S coupling.

Date: 2025
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DOI: 10.1038/s41467-025-63450-x

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