Concentration Optimization of Localized Cu0 and Cu+ on Cu-Based Electrodes for Improving Electrochemical Generation of Ethanol from Carbon Dioxide

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Abstract

Copper-based electrodes can catalyze electroreduction of CO2 to two-carbon products. However, obtaining a specific product with high efficiency depends on the oxidation state of Cu for the Cu-based materials. In this study, Cu-based electrodes were prepared on fluorinated tin oxide (FTO) using the one-step electrodeposition method. These electrodes were used as efficient electrocatalysts for CO2 reduction to ethanol. The concentration ratio of Cu0 and Cu+ on the electrodes was precisely modulated by adding monoethanolamine (MEA). The results of spectroscopic characterization showed that the concentration ratio of localized Cu+ and Cu0 (Cu+/Cu0) on the Cu-based electrodes was controlled from 1.24/1 to 1.54/1 by regulating the amount of MEA. It was found that the electrode exhibited the best electrochemical efficiency and ethanol production in the CO2 reduction reaction at the optimal concentration ratio Cu+/Cu0 of 1.42/1. The maximum faradaic efficiencies of ethanol and C2 were 48% and 77%, respectively, at the potential of −0.6 V vs. a reversible hydrogen electrode (RHE). Furthermore, the optimal concentration ratio of Cu+/Cu0 achieved the balance between Cu+ and Cu0 with the most favorable free energy for the formation of *CO intermediate. The stable existence of the *CO intermediate significantly contributed to the formation of the C–C bond for ethanol production.

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Lu, H., Wang, G., Zhou, Y., Wotango, A. S., Wu, J., Meng, Q., & Li, P. (2022). Concentration Optimization of Localized Cu0 and Cu+ on Cu-Based Electrodes for Improving Electrochemical Generation of Ethanol from Carbon Dioxide. International Journal of Molecular Sciences, 23(16). https://doi.org/10.3390/ijms23169373

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