The DOI matches its Crossref record; 10 of the 10 references it cites were found in a registry or an index.
Tuning the Selectivity of Carbon Dioxide Electroreduction toward Ethanol on Oxide-Derived CuxZn Catalysts
Abstract
The electrochemical reduction of carbon dioxide (CO 2 ) to ethanol (C 2 H 5 OH) and ethylene (C 2 H 4 ) using renewable electricity is a viable method for the production of these commercially vital chemicals. Copper (Cu) and its oxides are by far the most effective electrocatalysts for this purpose. However, the formation of ethanol using these catalysts is generally less favored in comparison to that of ethylene. In this work, we demonstrate that the selectivity of CO 2 reduction toward ethanol could be tuned by introducing a cocatalyst to generate an in situ source of mobile CO reactant. Cu-based oxides with different amounts of Zn dopants (Cu, Cu 10 Zn, Cu 4 Zn, and Cu 2 Zn) were prepared and used as catalysts under ambient pressure in aqueous 0.1 M KHCO 3 electrolyte. By varying the amount of Zn in the bimetallic catalysts, we found that the selectivity of ethanol versus ethylene production, defined by the ratio of their Faradaic efficiencies (FE ethanol /FE ethylene ), could be tuned by a factor of up to ∼12.5. Ethanol formation was maximized on Cu 4 Zn at −1.05 V vs RHE, with a remarkable Faradaic efficiency and current density of 29.1% and −8.2 mA/cm 2, respectively. The Cu 4 Zn catalyst was also catalytically stable for the production of ethanol for at least 5 h. The importance of Zn as a CO-producing site was demonstrated by performing CO 2 reduction on Cu–Ni and Cu–Ag bimetallic catalysts. Operando Raman spectroscopy revealed that the as-deposited Cu-based oxide films were reduced to the metallic state during CO 2 reduction, after which only signals belonging to CO adsorbed on Cu sites were recorded. This showed that the reduction of CO 2 probably occurred on metallic sites rather than on metal oxides. A two-site mechanism to rationalize the selective reduction of CO 2 to ethanol is proposed and discussed.
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Citations
Cites
New insights into the electrochemical reduction of carbon dioxide on metallic copper surfaces
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Electrocatalytic Conversion of Carbon Dioxide to Methane and Methanol on Transition Metal Surfaces
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Highly selective plasma-activated copper catalysts for carbon dioxide reduction to ethylene
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Self-citationProbing the Active Surface Sites for CO Reduction on Oxide-Derived Copper Electrocatalysts
Verdaguer-Casadevall, A., Li, C. W., Johansson, T. P., Scott, S. B., McKeown, J. T., Kumar, M., Stephens, I. E. L., Kanan, M. W., & Chorkendorff, I. (2015) · Journal of the American Chemical Society · doi:10.1021/jacs.5b06227 · Cited by 645
One-step electrosynthesis of ethylene and ethanol from CO2 in an alkaline electrolyzer
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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
What would it take for renewably powered electrosynthesis to displace petrochemical processes?
De Luna, P., Hahn, C., Higgins, D., Jaffer, S. A., Jaramillo, T. F., & Sargent, E. H. (2019) · Science · doi:10.1126/science.aav3506 · Cited by 3,052
Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels
Birdja, Y. Y., Pérez-Gallent, E., Figueiredo, M. C., Göttle, A. J., Calle-Vallejo, F., & Koper, M. T. M. (2019) · Nature Energy · doi:10.1038/s41560-019-0450-y · Cited by 2,747
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
General Techno-Economic Analysis of CO 2 Electrolysis Systems
Jouny, M., Luc, W., & Jiao, F. (2018) · Industrial & Engineering Chemistry Research · doi:10.1021/acs.iecr.7b03514 · Cited by 1,628
Metadata
- Authors
- Ren, D., Ang, B. S.-H., & Yeo, B. S.
- Venue
- ACS Catalysis
- Publisher
- American Chemical Society (ACS)
- Published
- 2016-11-09
- Volume
- 6
- Issue
- 12
- Pages
- 8239-8247
- ISSN
- 2155-5435 (ISSN-L)
- OpenAlex
- W2552233834
- Cited by
- 721
- References
- 10
- FWCI
- 12.96
- Type
- journal article
- Language
- en
- Open access
- closed
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