Journal of the American Chemical Society, volume 139, issue 10, pages 3774-3783
The Central Role of Bicarbonate in the Electrochemical Reduction of Carbon Dioxide on Gold
Marco Dunwell
1
,
Q Lu
1, 2
,
Jeffrey M Heyes
1
,
Jonathan Rosen
1
,
Jingguang Chen
2
,
Yushan Yan
1
,
Feng Jiao
1
,
1
Center
for Catalytic Science and Technology, Department of Chemical and Biomolecular
Engineering, University of Delaware, Newark, Delaware 19716, United States
|
Publication type: Journal Article
Publication date: 2017-03-06
Quartile SCImago
Q1
Quartile WOS
Q1
Impact factor: 15
ISSN: 00027863, 15205126
General Chemistry
Catalysis
Biochemistry
Colloid and Surface Chemistry
Abstract
Much effort has been devoted in the development of efficient catalysts for electrochemical reduction of CO2. Molecular level understanding of electrode-mediated process, particularly the role of bicarbonate in increasing CO2 reduction rates, is still lacking due to the difficulty of directly probing the electrochemical interface. We developed a protocol to observe normally invisible reaction intermediates with a surface enhanced spectroscopy by applying square-wave potential profiles. Further, we demonstrate that bicarbonate, through equilibrium exchange with dissolved CO2, rather than the supplied CO2, is the primary source of carbon in the CO formed at the Au electrode by a combination of in situ spectroscopic, isotopic labeling, and mass spectroscopic investigations. We propose that bicarbonate enhances the rate of CO production on Au by increasing the effective concentration of dissolved CO2 near the electrode surface through rapid equilibrium between bicarbonate and dissolved CO2.
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Citations by publishers
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160
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American Chemical Society (ACS)
145 publications, 29.12%
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1 publication, 0.2%
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1 publication, 0.2%
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IEEE
1 publication, 0.2%
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- We do not take into account publications without a DOI.
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Dunwell M. et al. The Central Role of Bicarbonate in the Electrochemical Reduction of Carbon Dioxide on Gold // Journal of the American Chemical Society. 2017. Vol. 139. No. 10. pp. 3774-3783.
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Dunwell M., Lu Q., Heyes J. M., Rosen J., Chen J., Yan Y., Jiao F., Xu B. The Central Role of Bicarbonate in the Electrochemical Reduction of Carbon Dioxide on Gold // Journal of the American Chemical Society. 2017. Vol. 139. No. 10. pp. 3774-3783.
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TY - JOUR
DO - 10.1021/jacs.6b13287
UR - https://doi.org/10.1021/jacs.6b13287
TI - The Central Role of Bicarbonate in the Electrochemical Reduction of Carbon Dioxide on Gold
T2 - Journal of the American Chemical Society
AU - Dunwell, Marco
AU - Heyes, Jeffrey M
AU - Jiao, Feng
AU - Xu, Bingjun
AU - Lu, Q
AU - Rosen, Jonathan
AU - Chen, Jingguang
AU - Yan, Yushan
PY - 2017
DA - 2017/03/06 00:00:00
PB - American Chemical Society (ACS)
SP - 3774-3783
IS - 10
VL - 139
SN - 0002-7863
SN - 1520-5126
ER -
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@article{2017_Dunwell,
author = {Marco Dunwell and Jeffrey M Heyes and Feng Jiao and Bingjun Xu and Q Lu and Jonathan Rosen and Jingguang Chen and Yushan Yan},
title = {The Central Role of Bicarbonate in the Electrochemical Reduction of Carbon Dioxide on Gold},
journal = {Journal of the American Chemical Society},
year = {2017},
volume = {139},
publisher = {American Chemical Society (ACS)},
month = {mar},
url = {https://doi.org/10.1021/jacs.6b13287},
number = {10},
pages = {3774--3783},
doi = {10.1021/jacs.6b13287}
}
Cite this
MLA
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Dunwell, Marco, et al. “The Central Role of Bicarbonate in the Electrochemical Reduction of Carbon Dioxide on Gold.” Journal of the American Chemical Society, vol. 139, no. 10, Mar. 2017, pp. 3774-3783. https://doi.org/10.1021/jacs.6b13287.