Cited by 250CO2 Reduction Techniques and CatalystsElectrocatalysts for Energy ConversionCatalysts for Methane Reforming

Effects of Anion Identity and Concentration on Electrochemical Reduction of CO 2

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Resasco, Joaquin, Lum, Yanwei, Clark, Ezra, Zeledon, Jose Zamora, Bell, Alexis T.·2018·ChemElectroChem

Abstract

The electrochemical reduction of CO 2 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 CO 2 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 CO 2 over Cu. It was demonstrated that the composition and concentration of electrolyte anions has relatively little effect on the formation of CO, HCOO − , C 2 H 4 , and CH 3 CH 2 OH, but has a significant effect on the formation of H 2 and CH 4 . 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 H 2 and CH 4 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 H 2 and CH 4 . 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 p K a of the buffering anion.

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Authors
Resasco, J., Lum, Y., Clark, E., Zeledon, J. Z., & Bell, A. T.
Affiliations
  • Lawrence Berkeley National Laboratory (US)
  • Department of Chemical Engineering University of California Berkeley, CA 94720
Corresponding author
Bell, Alexis T.
Venue
ChemElectroChem
Publisher
Wiley
Published
2018-02-12
Volume
5
Issue
7
Pages
1064-1072
ISSN
2196-0216 (ISSN-L)
OpenAlex
W2790215394
Cited by
250
References
42
Citations by year
2026: 25 · 2025: 38 · 2024: 25 · 2023: 29 · 2022: 40 · 2021: 32 · 2020: 27 · 2019: 20 · 2018: 14
FWCI
5.37
Type
journal article
Language
en
Open access
Locations
  • ChemElectroChem (publishedVersion)
  • OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
  • eScholarship (California Digital Library) (submittedVersion)
Funders
U.S. Department of Energy (DE-SC0004993)
Topics
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
  • Physical Sciences › Chemical Engineering › Catalysis › Catalysts for Methane Reforming
Keywords
electrochemical CO2 reduction, electrolyte anions, bicarbonate buffer, copper electrode, hydrogen production, methane production, surface pH, hydrogen donation, continuum model, product selectivity

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