The DOI matches its Crossref record; 8 of the 8 references it cites were found in a registry or an index.
Electrochemical Reduction of CO2 Using Copper Single-Crystal Surfaces: Effects of CO* Coverage on the Selective Formation of Ethylene
Abstract
Copper oxide-derived Cu catalysts are known to exhibit enhanced energetic efficiencies and selectivities towards the reduction of carbon dioxide to commercially vital C 2 products such as ethylene (C 2 H 4 ). However, the cause of this selectivity is not fully understood. In this work, we elucidated a fundamental reason underlying the selectivity of CO 2 reduction toward C 2 products by studying its reactivity on Cu(100), Cu(111), and Cu(110) single-crystal surfaces. A combination of cyclic and linear sweep voltammetries, chronoamperometry, online gas chromatography, 1 H nuclear magnetic resonance spectroscopy, and density functional theory (DFT) calculations was employed for this end. A wide range of electrochemical potentials from −0.28 to −1.25 V versus the reversible hydrogen electrode was investigated. Aqueous 0.1 M KHCO 3 was used as the electrolyte. We report here two general trends on Cu 2 O-derived Cu and Cu single-crystal surfaces: (i) the onset potential for the formation of C 2 H 4 always starts 300–400 mV more negative than the onset potential for CO evolution, and (ii) C 2 H 4 was formed only after a significant amount of CO gas was produced. Among the single-crystal surfaces investigated, Cu(100) required the lowest overpotential to reduce CO 2 to C 2 H 4 . These observations were rationalized using DFT simulations. Of the three single-crystal surfaces modeled, the dimerization of two CO* molecules on Cu(100) exhibited the lowest energy barrier, and this barrier can be further lowered with higher CO* coverages. The application of our observed experimental trends to other previously reported Cu-based systems strongly suggests that a high surface coverage of CO* is central for the selective formation of C 2 H 4 .
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Cites
How copper catalyzes the electroreduction of carbon dioxide into hydrocarbon fuels
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New insights into the electrochemical reduction of carbon dioxide on metallic copper surfaces
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Theoretical Considerations on the Electroreduction of CO to C 2 Species on Cu(100) Electrodes
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Self-citationGrain-Boundary-Dependent CO 2 Electroreduction Activity
Feng, X., Jiang, K., Fan, S., & Kanan, M. W. (2015) · Journal of the American Chemical Society · doi:10.1021/ja5130513 · Cited by 694
Competition between CO 2 Reduction and H 2 Evolution on Transition-Metal Electrocatalysts
Zhang, Y.-J., Sethuraman, V., Michalsky, R., & Peterson, A. A. (2014) · ACS Catalysis · doi:10.1021/cs5012298 · Cited by 509
Subsurface Oxygen in Oxide-Derived Copper Electrocatalysts for Carbon Dioxide Reduction
Eilert, A., Cavalca, F., Roberts, F. S., Osterwalder, J., Liu, C., Favaro, M., Crumlin, E. J., Ogasawara, H., Friebel, D., Pettersson, L. G. M., et al. (2017) · The Journal of Physical Chemistry Letters · doi:10.1021/acs.jpclett.6b02273 · Cited by 443
Cited by
Progress and perspectives of electrochemical CO2 reduction on copper in aqueous electrolyte
Nitopi, S., Bertheussen, E., Scott, S. B., Liu, X., Engstfeld, A. K., Horch, S., Seger, B., Stephens, I. E. L., Chan, K., Hahn, C., et al. (2019) · Chemical Reviews · doi:10.1021/acs.chemrev.8b00705 · Cited by 5,223
CO 2 electroreduction to ethylene via hydroxide-mediated copper catalysis at an abrupt interface
Dinh, C.-T., Burdyny, T., Kibria, M. G., Seifitokaldani, A., Gabardo, C. M., García de Arquer, F. P., Kiani, A., Edwards, J. P., De Luna, P., Bushuyev, O. S., et al. (2018) · Science · doi:10.1126/science.aas9100 · Cited by 2,515
Ma, W., Xie, S., Liu, T., Fan, Q., Ye, J., Sun, F., Jiang, Z., Zhang, Q., Cheng, J., & Wang, Y. (2020) · Nature Catalysis · doi:10.1038/s41929-020-0450-0 · Cited by 1,468
Industrial carbon dioxide capture and utilization: state of the art and future challenges
Gao, W., Liang, S., Wang, R., Jiang, Q., Zhang, Y., Zheng, Q., Xie, B., Toe, C. Y., Zhu, X., Wang, J., et al. (2020) · Chemical Society Reviews · doi:10.1039/d0cs00025f · Cited by 1,388
Designing materials for electrochemical carbon dioxide recycling
Ross, M. B., De Luna, P., Li, Y., Dinh, C.-T., Kim, D., Yang, P., & Sargent, E. H. (2019) · Nature Catalysis · doi:10.1038/s41929-019-0306-7 · Cited by 1,302
Metadata
- Authors
- Huang, Y., Handoko, A. D., Hirunsit, P., & Yeo, B. S.
- Venue
- ACS Catalysis
- Publisher
- American Chemical Society (ACS)
- Published
- 2017-02-06
- Volume
- 7
- Issue
- 3
- Pages
- 1749-1756
- ISSN
- 2155-5435 (ISSN-L)
- OpenAlex
- W2586083027
- Cited by
- 685
- References
- 8
- FWCI
- 14.80
- Type
- journal article
- Language
- en
- Open access
- closed
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