Effects of Anion Identity and Concentration on Electrochemical Reduction of CO2
Abstract
The electrochemical reduction of CO2 is known to be influenced by the concentration and identity of the anionic species in the electrolyte; however, a full understanding of this phenomenon has not been developed. Here, we present the results of experimental and computational studies aimed at understanding the role of electrolyte anions on the reduction of CO2 over Cu surfaces. Experimental studies were performed to show the effects of bicarbonate buffer concentration and the composition of other buffering anions on the partial currents of the major products formed by reduction of CO2 over Cu. It was demonstrated that the composition and concentration of electrolyte anions has relatively little effect on the formation of CO, HCOO-, C2H4, and CH3CH2OH, but has a significant effect on the formation of H2 and CH4. Continuum modeling was used to assess the effects of buffering anions on the pH at the electrode surface. The influence of pH on the activity of Cu for producing H2 and CH4 was also considered. Changes in the pH near the electrode surface were insufficient to explain the differences in activity and selectivity observed with changes in anion buffering capacity observed for the formation of H2 and CH4. Therefore, it ismore »
- Authors:
-
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1571098
- Alternate Identifier(s):
- OSTI ID: 1420191
- Grant/Contract Number:
- AC02-05CH11231; SC0004993; DGE-0802270
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ChemElectroChem
- Additional Journal Information:
- Journal Volume: 5; Journal Issue: 7; Journal ID: ISSN 2196-0216
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Resasco, Joaquin, Lum, Yanwei, Clark, Ezra, Zeledon, Jose Zamora, and Bell, Alexis T. Effects of Anion Identity and Concentration on Electrochemical Reduction of CO2. United States: N. p., 2018.
Web. doi:10.1002/celc.201701316.
Resasco, Joaquin, Lum, Yanwei, Clark, Ezra, Zeledon, Jose Zamora, & Bell, Alexis T. Effects of Anion Identity and Concentration on Electrochemical Reduction of CO2. United States. https://doi.org/10.1002/celc.201701316
Resasco, Joaquin, Lum, Yanwei, Clark, Ezra, Zeledon, Jose Zamora, and Bell, Alexis T. Mon .
"Effects of Anion Identity and Concentration on Electrochemical Reduction of CO2". United States. https://doi.org/10.1002/celc.201701316. https://www.osti.gov/servlets/purl/1571098.
@article{osti_1571098,
title = {Effects of Anion Identity and Concentration on Electrochemical Reduction of CO2},
author = {Resasco, Joaquin and Lum, Yanwei and Clark, Ezra and Zeledon, Jose Zamora and Bell, Alexis T.},
abstractNote = {The electrochemical reduction of CO2 is known to be influenced by the concentration and identity of the anionic species in the electrolyte; however, a full understanding of this phenomenon has not been developed. Here, we present the results of experimental and computational studies aimed at understanding the role of electrolyte anions on the reduction of CO2 over Cu surfaces. Experimental studies were performed to show the effects of bicarbonate buffer concentration and the composition of other buffering anions on the partial currents of the major products formed by reduction of CO2 over Cu. It was demonstrated that the composition and concentration of electrolyte anions has relatively little effect on the formation of CO, HCOO-, C2H4, and CH3CH2OH, but has a significant effect on the formation of H2 and CH4. Continuum modeling was used to assess the effects of buffering anions on the pH at the electrode surface. The influence of pH on the activity of Cu for producing H2 and CH4 was also considered. Changes in the pH near the electrode surface were insufficient to explain the differences in activity and selectivity observed with changes in anion buffering capacity observed for the formation of H2 and CH4. Therefore, it is proposed that these differences are the result of the ability of buffering anions to donate hydrogen directly to the electrode surface and in competition with water. The effectiveness of buffering anions to serve as hydrogen donors is found to increase with decreasing pKa of the buffering anion.},
doi = {10.1002/celc.201701316},
journal = {ChemElectroChem},
number = 7,
volume = 5,
place = {United States},
year = {Mon Feb 12 00:00:00 EST 2018},
month = {Mon Feb 12 00:00:00 EST 2018}
}
Web of Science
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