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Competition between CO2 Reduction and Hydrogen Evolution on a Gold Electrode under Well-Defined Mass Transport Conditions
Open accessAbstract
(CO2RR) to CO. However, the concomitant hydrogen evolution reaction (HER) remains unavoidable under aqueous conditions. In this work, a rotating ring disk electrode (RRDE) setup has been developed to study quantitatively the role of mass transport in the competition between these two reactions on the Au surface in 0.1 M bicarbonate electrolyte. Interestingly, while the faradaic selectivity for CO formation was found to increase with enhanced mass transport (from 67% to 83%), this effect is not due to an enhancement of the CO2RR rate. Remarkably, the inhibition of the competing HER from water reduction with increasing disk rotation rate is responsible for the enhanced CO2RR selectivity. This can be explained by the observation that, on the Au electrode, water reduction improves with more alkaline pH. As a result, the decrease in the local alkalinity near the electrode surface with enhanced mass transport suppresses HER due to the water reduction. Our study shows that controlling the local pH by mass transport conditions can tune the HER rate, in turn regulating the CO2RR and HER competition in the general operating potential window for CO2RR (-0.4 to -1 V vs RHE).
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Cites
Combining theory and experiment in electrocatalysis: Insights into materials design
Seh, Z. W., Kibsgaard, J., Dickens, C. F., Chorkendorff, I., Nørskov, J. K., & Jaramillo, T. F. (2017) · Science · doi:10.1126/science.aad4998 · Cited by 12,114
Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels
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Grain-Boundary-Dependent CO 2 Electroreduction Activity
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Effects of Anion Identity and Concentration on Electrochemical Reduction of CO 2
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Tuning of CO2 Reduction Selectivity on Metal Electrocatalysts
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Precious Metal Free Hydrogen Evolution Catalyst Design and Application
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Electrified water treatment: fundamentals and roles of electrode materials
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Metadata
- Authors
- Goyal, A., Marcandalli, G., Mints, V. A., & Koper, M. T. M.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2020-02-10
- Volume
- 142
- Issue
- 9
- Pages
- 4154-4161
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W3005814135
- Cited by
- 637
- References
- 6
- FWCI
- 13.97
- Type
- journal article
- Language
- en
- Open access
- hybrid
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