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Synergistic copper-manganese oxide electrocatalysts for CO2 conversion to CO
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DOI：10.1007/s10853-026-13380-w.png)
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Abstract
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CO is a key product of CO2 electroreduction (CO2ER) and an important feedstock for the production of hydrocarbons and alcohols. Herein, we synthesized electrocatalysts by growing Cu nanocluster on manganese oxide (Cun-Mn3O4) for CO2ER. In 0.5 M KHCO3 electrolyte using an H-cell, the optimized Cu0.4-Mn3O4 achieved a Faradaic efficiency for CO (FECO) of 88.5 ± 2.3% and a current density of 14.3 ± 0.2 mA cm−2 at − 0.6 V vs. RHE, while substantially suppressing the hydrogen evolution reaction (HER). The better performance was due to the electrons transferred from Mn to CO2 by Cu as a shuttle and anchored Cu nanoclusters shifted the d-band center toward the Fermi level, which was more conducive to the intermediate formation. In situ electrochemical attenuated total internal reflectance (EC-ATR) spectroscopy and density functional theory (DFT) calculations revealed the *COOH intermediate (1399 cm⁻1) along the CO2 → *COOH → *CO → CO pathway. Moreover, the DFT calculations further demonstrated the Gibbs free energy barrier (ΔG) of the key steps in the CO2ER pathway and the corresponding intermediate configurations, which were used to reveal the relationship between the catalyst structure and CO2ER performance. The design of the metal/metal oxide electrocatalyst in this study provides a new perspective for the highly selective reduction of CO2 to CO.
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