Combined high alkalinity and pressurization enable efficient CO2 electroreduction to CO

Christine M. Gabardo; Ali Seifitokaldani; Jonathan P. Edwards; Cao Thang Dinh; Thomas Burdyny; Md Golam Kibria; Colin P. O'Brien; Edward H. Sargent; David Sinton

doi:10.1039/c8ee01684d

Combined high alkalinity and pressurization enable efficient CO₂ electroreduction to CO

Christine M. Gabardo, Ali Seifitokaldani, Jonathan P. Edwards, Cao Thang Dinh, Thomas Burdyny, Md Golam Kibria, Colin P. O'Brien, Edward H. Sargent, David Sinton^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

250 Scopus citations

Abstract

The electroreduction of carbon dioxide (CO₂) to carbon monoxide (CO) is a promising strategy to utilize CO₂ emissions while generating a high value product. Commercial CO₂ electroreduction systems will require high current densities (>100 mA cm^-2) as well as improved energetic efficiencies (EEs), achieved via high CO selectivity and lowered applied potentials. Here we report a silver (Ag)-based system that exhibits the lowest overpotential among CO₂-to-CO electrolyzers operating at high current densities, 300 mV at 300 mA cm^-2, with near unity selectivity. We achieve these improvements in voltage efficiency and selectivity via operation in a highly alkaline reaction environment (which decreases overpotentials) and system pressurization (which suppresses the generation of alternative CO₂ reduction products), respectively. In addition, we report a new record for the highest half-cell EE (>80%) for CO production at 300 mA cm^-2.

Original language	English (US)
Pages (from-to)	2531-2539
Number of pages	9
Journal	Energy and Environmental Science
Volume	11
Issue number	9
DOIs	https://doi.org/10.1039/c8ee01684d
State	Published - Sep 2018

Funding

The authors acknowledge support from the Natural Sciences and Engineering Research Council (NSERC), the Government of Ontario through the Ontario Research Fund – Research Excellence program, and the Connaught Fund. X-ray spectroscopy measurements were performed at the Canadian Light Source (SXRMB beamline) and the authors thank Dr Y. Hu and Dr Q. Xiao for XAS support. The authors would like to thank Y. Wang, P. De Luna, D.-H. Nam, R. Q. Bermudez, and C.-S. Tan for their help with materials characterization. C. M. G. would like to thank NSERC for support in the form of a postdoctoral fellowship award. A. S. wishes to thank FRQNT for support in the form of postdoctoral fellowship award. J. P. E. thanks NSERC, Hatch and the Government of Ontario for their support through graduate scholarships. J. P. E. also thanks S. Verma and S. Bhargava at the Kenis Lab for helpful input on flow cell testing. T. B. thanks Hatch for a Graduate Scholarship for Sustainable Energy Research. M. K. acknowledges Banting postdoctoral fellowship from Govt. of Canada.

ASJC Scopus subject areas

Environmental Chemistry
Renewable Energy, Sustainability and the Environment
Nuclear Energy and Engineering
Pollution

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1039/c8ee01684d

Cite this

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title = "Combined high alkalinity and pressurization enable efficient CO2 electroreduction to CO",

abstract = "The electroreduction of carbon dioxide (CO2) to carbon monoxide (CO) is a promising strategy to utilize CO2 emissions while generating a high value product. Commercial CO2 electroreduction systems will require high current densities (>100 mA cm-2) as well as improved energetic efficiencies (EEs), achieved via high CO selectivity and lowered applied potentials. Here we report a silver (Ag)-based system that exhibits the lowest overpotential among CO2-to-CO electrolyzers operating at high current densities, 300 mV at 300 mA cm-2, with near unity selectivity. We achieve these improvements in voltage efficiency and selectivity via operation in a highly alkaline reaction environment (which decreases overpotentials) and system pressurization (which suppresses the generation of alternative CO2 reduction products), respectively. In addition, we report a new record for the highest half-cell EE (>80%) for CO production at 300 mA cm-2.",

author = "Gabardo, {Christine M.} and Ali Seifitokaldani and Edwards, {Jonathan P.} and Dinh, {Cao Thang} and Thomas Burdyny and Kibria, {Md Golam} and O'Brien, {Colin P.} and Sargent, {Edward H.} and David Sinton",

note = "Funding Information: The authors acknowledge support from the Natural Sciences and Engineering Research Council (NSERC), the Government of Ontario through the Ontario Research Fund – Research Excellence program, and the Connaught Fund. X-ray spectroscopy measurements were performed at the Canadian Light Source (SXRMB beamline) and the authors thank Dr Y. Hu and Dr Q. Xiao for XAS support. The authors would like to thank Y. Wang, P. De Luna, D.-H. Nam, R. Q. Bermudez, and C.-S. Tan for their help with materials characterization. C. M. G. would like to thank NSERC for support in the form of a postdoctoral fellowship award. A. S. wishes to thank FRQNT for support in the form of postdoctoral fellowship award. J. P. E. thanks NSERC, Hatch and the Government of Ontario for their support through graduate scholarships. J. P. E. also thanks S. Verma and S. Bhargava at the Kenis Lab for helpful input on flow cell testing. T. B. thanks Hatch for a Graduate Scholarship for Sustainable Energy Research. M. K. acknowledges Banting postdoctoral fellowship from Govt. of Canada. Publisher Copyright: {\textcopyright} 2018 The Royal Society of Chemistry.",

year = "2018",

month = sep,

doi = "10.1039/c8ee01684d",

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AU - Gabardo, Christine M.

AU - Seifitokaldani, Ali

AU - Edwards, Jonathan P.

AU - Dinh, Cao Thang

AU - Burdyny, Thomas

AU - Kibria, Md Golam

AU - O'Brien, Colin P.

AU - Sargent, Edward H.

AU - Sinton, David

N1 - Funding Information: The authors acknowledge support from the Natural Sciences and Engineering Research Council (NSERC), the Government of Ontario through the Ontario Research Fund – Research Excellence program, and the Connaught Fund. X-ray spectroscopy measurements were performed at the Canadian Light Source (SXRMB beamline) and the authors thank Dr Y. Hu and Dr Q. Xiao for XAS support. The authors would like to thank Y. Wang, P. De Luna, D.-H. Nam, R. Q. Bermudez, and C.-S. Tan for their help with materials characterization. C. M. G. would like to thank NSERC for support in the form of a postdoctoral fellowship award. A. S. wishes to thank FRQNT for support in the form of postdoctoral fellowship award. J. P. E. thanks NSERC, Hatch and the Government of Ontario for their support through graduate scholarships. J. P. E. also thanks S. Verma and S. Bhargava at the Kenis Lab for helpful input on flow cell testing. T. B. thanks Hatch for a Graduate Scholarship for Sustainable Energy Research. M. K. acknowledges Banting postdoctoral fellowship from Govt. of Canada. Publisher Copyright: © 2018 The Royal Society of Chemistry.

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N2 - The electroreduction of carbon dioxide (CO2) to carbon monoxide (CO) is a promising strategy to utilize CO2 emissions while generating a high value product. Commercial CO2 electroreduction systems will require high current densities (>100 mA cm-2) as well as improved energetic efficiencies (EEs), achieved via high CO selectivity and lowered applied potentials. Here we report a silver (Ag)-based system that exhibits the lowest overpotential among CO2-to-CO electrolyzers operating at high current densities, 300 mV at 300 mA cm-2, with near unity selectivity. We achieve these improvements in voltage efficiency and selectivity via operation in a highly alkaline reaction environment (which decreases overpotentials) and system pressurization (which suppresses the generation of alternative CO2 reduction products), respectively. In addition, we report a new record for the highest half-cell EE (>80%) for CO production at 300 mA cm-2.

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