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Title: Engineering Catalyst–Electrolyte Microenvironments to Optimize the Activity and Selectivity for the Electrochemical Reduction of CO2 on Cu and Ag

Abstract

We report the electrochemical reduction of carbon dioxide (CO2R) driven by renewably generated electricity (e.g., solar and wind) offers a promising means for reusing the CO2 released during the production of cement, steel, and aluminum as well as the production of ammonia and methanol. If CO2 could be removed from the atmosphere at acceptable costs (i.e., <$100/t of CO2), then CO2R could be used to produce carbon-containing chemicals and fuels in a fully sustainable manner. Economic considerations dictate that CO2R current densities must be in the range of 0.1 to 1 A/cm2 and selectivity toward the targeted product must be high in order to minimize separation costs. Industrially relevant operating conditions can be achieved by using gas diffusion electrodes (GDEs) to maximize the transport of species to and from the cathode and combining such electrodes with a solid-electrolyte membrane by eliminating the ohmic losses associated with liquid electrolytes. Additionally, high product selectivity can be attained by careful tuning of the microenvironment near the catalyst surface (e.g., the pH, the concentrations of CO2 and H2O, and the identities of the cations in the double layer adjacent to the catalyst surface).

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1];  [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [1]
  1. University of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. 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), Basic Energy Sciences (BES); National Science Foundation (NSF); National Defense Science and Engineering Graduate Fellowship; National Research Foundation of Korea (NRF)
OSTI Identifier:
1877098
Grant/Contract Number:  
SC0021266; AC02-05CH11231; DGE-1752814; NRF-2021R1A6A3A14044966
Resource Type:
Accepted Manuscript
Journal Name:
Accounts of Chemical Research
Additional Journal Information:
Journal Volume: 55; Journal Issue: 4; Journal ID: ISSN 0001-4842
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Bui, Justin C., Kim, Chanyeon, King, Alex J., Romiluyi, Oyinkansola, Kusoglu, Ahmet, Weber, Adam Z., and Bell, Alexis T. Engineering Catalyst–Electrolyte Microenvironments to Optimize the Activity and Selectivity for the Electrochemical Reduction of CO2 on Cu and Ag. United States: N. p., 2022. Web. doi:10.1021/acs.accounts.1c00650.
Bui, Justin C., Kim, Chanyeon, King, Alex J., Romiluyi, Oyinkansola, Kusoglu, Ahmet, Weber, Adam Z., & Bell, Alexis T. Engineering Catalyst–Electrolyte Microenvironments to Optimize the Activity and Selectivity for the Electrochemical Reduction of CO2 on Cu and Ag. United States. https://doi.org/10.1021/acs.accounts.1c00650
Bui, Justin C., Kim, Chanyeon, King, Alex J., Romiluyi, Oyinkansola, Kusoglu, Ahmet, Weber, Adam Z., and Bell, Alexis T. Tue . "Engineering Catalyst–Electrolyte Microenvironments to Optimize the Activity and Selectivity for the Electrochemical Reduction of CO2 on Cu and Ag". United States. https://doi.org/10.1021/acs.accounts.1c00650. https://www.osti.gov/servlets/purl/1877098.
@article{osti_1877098,
title = {Engineering Catalyst–Electrolyte Microenvironments to Optimize the Activity and Selectivity for the Electrochemical Reduction of CO2 on Cu and Ag},
author = {Bui, Justin C. and Kim, Chanyeon and King, Alex J. and Romiluyi, Oyinkansola and Kusoglu, Ahmet and Weber, Adam Z. and Bell, Alexis T.},
abstractNote = {We report the electrochemical reduction of carbon dioxide (CO2R) driven by renewably generated electricity (e.g., solar and wind) offers a promising means for reusing the CO2 released during the production of cement, steel, and aluminum as well as the production of ammonia and methanol. If CO2 could be removed from the atmosphere at acceptable costs (i.e., <$100/t of CO2), then CO2R could be used to produce carbon-containing chemicals and fuels in a fully sustainable manner. Economic considerations dictate that CO2R current densities must be in the range of 0.1 to 1 A/cm2 and selectivity toward the targeted product must be high in order to minimize separation costs. Industrially relevant operating conditions can be achieved by using gas diffusion electrodes (GDEs) to maximize the transport of species to and from the cathode and combining such electrodes with a solid-electrolyte membrane by eliminating the ohmic losses associated with liquid electrolytes. Additionally, high product selectivity can be attained by careful tuning of the microenvironment near the catalyst surface (e.g., the pH, the concentrations of CO2 and H2O, and the identities of the cations in the double layer adjacent to the catalyst surface).},
doi = {10.1021/acs.accounts.1c00650},
journal = {Accounts of Chemical Research},
number = 4,
volume = 55,
place = {United States},
year = {Tue Feb 01 00:00:00 EST 2022},
month = {Tue Feb 01 00:00:00 EST 2022}
}

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