The DOI matches its Crossref record; 82 of the 82 references it cites were found in a registry or an index.
In Situ Infrared Spectroscopic Evidence of Enhanced Electrochemical CO2 Reduction and C–C Coupling on Oxide-Derived Copper
Abstract
The reaction mechanism of CO 2 electroreduction on oxide-derived copper has not yet been unraveled even though high C 2+ Faradaic efficiencies are commonly observed on these surfaces. In this study, we aim to explore the effects of copper anodization on the adsorption of various CO 2 RR intermediates using in situ surface-enhanced infrared absorption spectroscopy (SEIRAS) on metallic and mildly anodized copper thin films. The in situ SEIRAS results show that the preoxidation process can significantly improve the overall CO 2 reduction activity by (1) enhancing CO 2 activation, (2) increasing CO uptake, and (3) promoting C–C coupling. First, the strong *COO – redshift indicates that the preoxidation process significantly enhances the first elementary step of CO 2 adsorption and activation. The rapid uptake of adsorbed *CO atop also illustrates how a high *CO coverage can be achieved in oxide-derived copper electrocatalysts. Finally, for the first time, we observed the formation of the *COCHO dimer on the anodized copper thin film. Using DFT calculations, we show how the presence of subsurface oxygen within the Cu lattice can improve the thermodynamics of C 2 product formation via the coupling of adsorbed *CO and *CHO intermediates. This study advances our understanding of the role of surface and subsurface conditions in improving the catalytic reaction kinetics and product selectivity of CO 2 reduction.
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Cites
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Metadata
- Authors
- Delmo, E. P., Wang, Y., Song, Y., Zhu, S., Zhang, H., Xu, H., Li, T., Jang, J., Kwon, Y., Wang, Y., & Shao, M.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2024-01-08
- Volume
- 146
- Issue
- 3
- Pages
- 1935-1945
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W4390685141
- Cited by
- 336
- References
- 82
- FWCI
- 22.20
- Type
- journal article
- Language
- en
- Open access
- closed
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- Delmo, E. P., Wang, Y., Song, Y., Zhu, S., Zhang, H., Xu, H., Li, T., Jang, J., Kwon, Y., Wang, Y., & Shao, M. (2024). In Situ Infrared Spectroscopic Evidence of Enhanced Electrochemical CO2 Reduction and C–C Coupling on Oxide-Derived Copper. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.3c08927
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