Effect of Gold Catalyst Surface Morphology on Wetting Behavior and Electrochemical CO2 Reduction Performance in a Large-Area Zero-Gap Gas Diffusion Electrolyzer
Abstract
We report catalyst surface area and wetting behavior are key factors in determining the performance of gas diffusion electrode (GDE) electrolyzers for electrochemical CO2 reduction. In this work, we report the integration of sub-1 μm thick nanoporous gold (npAu) catalyst coatings into a large-area (25 cm2) zero-gap electrolyzer. The npAu coatings were prepared by magnetron sputtering (MS) of thin AgAu alloy films on the microporous carbon layer of a gas diffusion layer (GDL) followed by Ag leaching. Compared to MS Au films of the same thickness, npAu catalyst coatings enable higher Faradaic efficiencies and improved catalyst stability for CO2-to-CO reduction with Faradaic efficiencies of up to 88% at 100 mA/cm2. For a 800 nm npAu coating, the device level energy efficiency for CO2 to CO conversion reaches 45% (52% for CO + H2) at 100 mA/cm2 with a single pass CO2 conversion efficiency of ~12%. Contact angle measurements reveal that npAu coatings provide a more hydrophobic electrode interface compared to MS Au coatings, suggesting that the more hydrophobic interfacial environment of npAu coatings helps mitigating electrode flooding which is associated with performance deterioration over time.
- Authors:
-
[1];
[1];
[1];
[3];
[3];
[1]
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
- Twelve Benefit Corporation, Berkeley, CA (United States)
- University of Pennsylvania, Philadelphia, PA (United States)
- Publication Date:
- Research Org.:
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Science Foundation (NSF)
- OSTI Identifier:
- 1902016
- Report Number(s):
- LLNL-JRNL-834289
Journal ID: ISSN 1932-7447; 1052662
- Grant/Contract Number:
- AC52-07NA27344; EE-0008327; TCF-20-20160; AC02-05CH11231; NNCI-1542153; DMR-1720530
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 126; Journal Issue: 46; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY; 36 MATERIALS SCIENCE; 30 DIRECT ENERGY CONVERSION; nanoporous gold; electrochemical CO2 reduction; dealloying; surface roughness; gas diffusion electrode; wetting behavior
Citation Formats
Qi, Zhen, Kashi, Ajay R., Buckley, Aya K., Miller, John S., Ye, Jianchao, Biener, Monika M., Foucher, Alexandre C., Stach, Eric A., Ma, Sichao, Kuhl, Kendra P., and Biener, Juergen. Effect of Gold Catalyst Surface Morphology on Wetting Behavior and Electrochemical CO2 Reduction Performance in a Large-Area Zero-Gap Gas Diffusion Electrolyzer. United States: N. p., 2022.
Web. doi:10.1021/acs.jpcc.2c03773.
Qi, Zhen, Kashi, Ajay R., Buckley, Aya K., Miller, John S., Ye, Jianchao, Biener, Monika M., Foucher, Alexandre C., Stach, Eric A., Ma, Sichao, Kuhl, Kendra P., & Biener, Juergen. Effect of Gold Catalyst Surface Morphology on Wetting Behavior and Electrochemical CO2 Reduction Performance in a Large-Area Zero-Gap Gas Diffusion Electrolyzer. United States. https://doi.org/10.1021/acs.jpcc.2c03773
Qi, Zhen, Kashi, Ajay R., Buckley, Aya K., Miller, John S., Ye, Jianchao, Biener, Monika M., Foucher, Alexandre C., Stach, Eric A., Ma, Sichao, Kuhl, Kendra P., and Biener, Juergen. Wed .
"Effect of Gold Catalyst Surface Morphology on Wetting Behavior and Electrochemical CO2 Reduction Performance in a Large-Area Zero-Gap Gas Diffusion Electrolyzer". United States. https://doi.org/10.1021/acs.jpcc.2c03773. https://www.osti.gov/servlets/purl/1902016.
@article{osti_1902016,
title = {Effect of Gold Catalyst Surface Morphology on Wetting Behavior and Electrochemical CO2 Reduction Performance in a Large-Area Zero-Gap Gas Diffusion Electrolyzer},
author = {Qi, Zhen and Kashi, Ajay R. and Buckley, Aya K. and Miller, John S. and Ye, Jianchao and Biener, Monika M. and Foucher, Alexandre C. and Stach, Eric A. and Ma, Sichao and Kuhl, Kendra P. and Biener, Juergen},
abstractNote = {We report catalyst surface area and wetting behavior are key factors in determining the performance of gas diffusion electrode (GDE) electrolyzers for electrochemical CO2 reduction. In this work, we report the integration of sub-1 μm thick nanoporous gold (npAu) catalyst coatings into a large-area (25 cm2) zero-gap electrolyzer. The npAu coatings were prepared by magnetron sputtering (MS) of thin AgAu alloy films on the microporous carbon layer of a gas diffusion layer (GDL) followed by Ag leaching. Compared to MS Au films of the same thickness, npAu catalyst coatings enable higher Faradaic efficiencies and improved catalyst stability for CO2-to-CO reduction with Faradaic efficiencies of up to 88% at 100 mA/cm2. For a 800 nm npAu coating, the device level energy efficiency for CO2 to CO conversion reaches 45% (52% for CO + H2) at 100 mA/cm2 with a single pass CO2 conversion efficiency of ~12%. Contact angle measurements reveal that npAu coatings provide a more hydrophobic electrode interface compared to MS Au coatings, suggesting that the more hydrophobic interfacial environment of npAu coatings helps mitigating electrode flooding which is associated with performance deterioration over time.},
doi = {10.1021/acs.jpcc.2c03773},
journal = {Journal of Physical Chemistry. C},
number = 46,
volume = 126,
place = {United States},
year = {Wed Nov 09 00:00:00 EST 2022},
month = {Wed Nov 09 00:00:00 EST 2022}
}
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