Authors
Putri Ramadhany, Peiqi Qiu, Thành Trần-Phú, Denny Gunawan, Bernt Johannessen, Rosalie K Hocking, Yan Jiao, Rose Amal, Rahman Daiyan
Published in
Advanced materials (Deerfield Beach, Fla.). Pages e75357. Oct 13, 2026. Epub Oct 13, 2026.
Abstract
Electrochemical C─N coupling of CO2 with nitrogen species offers a sustainable route to urea and related chemicals but is constrained under steady-state electrolysis by mismatched reaction kinetics. Here, pulsed oxidative-reductive electrolysis temporally coordinates CO2 reduction and NH3 oxidation, regulating the generation and coexistence of carbon- and nitrogen-derived intermediates. Co/CuNC, containing atomically dispersed Co and Cu sites within a nitrogen-doped carbon (NC), achieves a total C─N faradaic efficiency of 42 ± 4%, dominated by urea (20 ± 2%) and ethyl urea (16 ± 2%), with respective yield rates (YR) of 295 ± 25 and 50 ± 5 mmol h-1 gcat -1. In situ synchrotron x-ray absorption spectroscopy (XAS) reveals potential-dependent changes in Cu and Co oxidation states and coordination environments, while in situ infrared spectroscopy identifies pulse-regulated *CO and *NHx intermediates and suggests concurrent electrochemical and Wöhler-type pathways. Density functional theory calculations reveal complementary site functions: Cu favors *NH2 formation, whereas Co more strongly stabilizes *NHx and *CO intermediates, with *CO also accessible at Cu sites. These findings establish temporal coordination of reactant activation, intermediate populations, and active-site states as a mode-enabled strategy for accessing higher-order C─N products.
PMID:
42867457
Bibliographic data and abstract were imported from PubMed on 14 Oct 2026.
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