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Facilitating electrocatalytic CO2 reduction through electrolyte additives accompanied by activation of copper electrode with cyclic voltammetry

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Abstract

Electrode materials have an important impact on the efficiency and product selectivity of electrocatalytic CO2 reduction, and copper is favored as an electrode material capable of generating a variety of multicarbon products. However, its poor product selectivity limits its large-scale application. In order to regulate the selectivity to certain products, 1,2-cyclohexylenedinitrilotetraacetic acid (CyDTA) was employed as electrolyte additive to form Cu–N active sites by ligand chelation with copper, which improved the selectivity of CH4. Furthermore, the electrode modification was enhanced with activation using cyclic voltammetry (CV), and the results showed that the CV activation significantly strengthened the interaction between CyDTA and copper electrode, which led to the highest partial current density up to 9.3 mA cm−2 of CH4 in an H-type electrolytic cell at an electrode potential of − 1.0 V (vs. RHE). Under this condition, the Faradaic efficiency of CH4 was up to 74% and could be kept more than 50% after 8-h constant potential electrolysis. The results of this study provided a new strategy to improve the selectivity of CO2 reduction products with copper electrode, which can promote the wide application of electrocatalytic CO2 reduction process.

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Funding

This study received support from the National Natural Science Foundation of China (No. 51208299).

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Authors and Affiliations

  1. School of Environment & Architecture, University of Shanghai for Science & Technology, No. 516, Jungong Road, Shanghai, People’s Republic of China

    Zheng Yuan, Xinming Yang, Ling Wang, Junkai Zhao, Shiqi Chen, Yifan Liang, Yu Sun & Liang Li

  2. Shanghai Urban Construction Vocational College, Shanghai, 200438, People’s Republic of China

    Ya Gao

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  1. Zheng Yuan
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  2. Ya Gao
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  3. Xinming Yang
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  4. Ling Wang
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  8. Yu Sun
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Contributions

Z.Y. wrote the main manuscript text. Y.G., X.Y., L.W., and J.Z. prepared Figs. 1–7. S.C., Y.L., and Y.S. prepared the “Supplementary information.” L.L. revised the manuscript. All authors reviewed the manuscript.

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Correspondence to Liang Li.

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Yuan, Z., Gao, Y., Yang, X. et al. Facilitating electrocatalytic CO2 reduction through electrolyte additives accompanied by activation of copper electrode with cyclic voltammetry. Ionics 30, 2387–2396 (2024). https://doi.org/10.1007/s11581-024-05420-9

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