Effect of Gold Catalyst Surface Morphology on Wetting Behavior and Electrochemical CO2Reduction Performance in a Large-Area Zero-Gap Gas Diffusion Electrolyzer

Zhen Qi; Ajay R. Kashi; Aya K. Buckley; John S. Miller; Jianchao Ye; Monika M. Biener; Alexandre C. Foucher; Eric A. Stach; Sichao Ma; Kendra P. Kuhl; Juergen Biener

doi:10.1021/acs.jpcc.2c03773

Effect of Gold Catalyst Surface Morphology on Wetting Behavior and Electrochemical CO₂Reduction Performance in a Large-Area Zero-Gap Gas Diffusion Electrolyzer

Zhen Qi, Ajay R. Kashi, Aya K. Buckley, John S. Miller, Jianchao Ye, Monika M. Biener, Alexandre C. Foucher, Eric A. Stach, Sichao Ma, Kendra P. Kuhl, Juergen Biener

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

3 Scopus citations

Abstract

Catalyst surface area and wetting behavior are key factors in determining the performance of gas diffusion electrode (GDE) electrolyzers for electrochemical CO₂reduction. 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 CO₂to CO conversion reaches 45% (52% for CO + H₂) at 100 mA/cm²with a single pass CO₂conversion 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.

Original language	English
Pages (from-to)	19637-19646
Number of pages	10
Journal	Journal of Physical Chemistry C
Volume	126
Issue number	46
DOIs	https://doi.org/10.1021/acs.jpcc.2c03773
State	Published - Nov 24 2022
Externally published	Yes

Funding

This work was supported by the U.S. Department of Energy’s Office of Energy Efficiency and Renewable Energy (EERE) under the Advanced Manufacturing Office Next Generation R&D Projects Award DE-EE-0008327 and Office of Technology Transitions under Technology Commercialization Fund Award TCF-20-20160. The views expressed herein do not necessarily represent the views of the U.S. Department of Energy or the United States Government. The work was performed under the auspices of the US Department of Energy by LLNL under Contract DE-AC52-07NA27344. We are grateful for the nanofabrication and imaging facilities in the Molecular Foundry at the Lawrence Berkeley National Laboratory. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract DE-AC02-05CH11231. TEM experiments were also performed at the Nanoscale Characterization Facility, Singh Center for Nanotechnology at the University of Pennsylvania, supported by the National Science Foundation (NSF) National Nanotechnology Coordinated Infrastructure Program Grant NNCI-1542153. Additional support provided by the Laboratory for Research on the Structure of Matter (MRSEC) supported by the National Science Foundation (DMR-1720530).

Funders	Funder number
Laboratory for Research on the Structure of Matter
National Science Foundation	NNCI-1542153
U.S. Department of Energy
Office of Science
Office of Energy Efficiency and Renewable Energy	DE-EE-0008327
Basic Energy Sciences	DE-AC02-05CH11231
Lawrence Livermore National Laboratory	DE-AC52-07NA27344
Materials Research Science and Engineering Center, Harvard University	DMR-1720530
Office of Technology Transitions	TCF-20-20160

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10.1021/acs.jpcc.2c03773

Cite this

Qi, Z., Kashi, A. R., Buckley, A. K., Miller, J. S., Ye, J., Biener, M. M., Foucher, A. C., Stach, E. A., Ma, S., Kuhl, K. P., & Biener, J. (2022). Effect of Gold Catalyst Surface Morphology on Wetting Behavior and Electrochemical CO₂Reduction Performance in a Large-Area Zero-Gap Gas Diffusion Electrolyzer. Journal of Physical Chemistry C, 126(46), 19637-19646. https://doi.org/10.1021/acs.jpcc.2c03773

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abstract = "Catalyst surface area and wetting behavior are key factors in determining the performance of gas diffusion electrode (GDE) electrolyzers for electrochemical CO2reduction. 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 CO2to CO conversion reaches 45% (52% for CO + H2) at 100 mA/cm2with a single pass CO2conversion 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.",

author = "Zhen Qi and Kashi, {Ajay R.} and Buckley, {Aya K.} and Miller, {John S.} and Jianchao Ye and Biener, {Monika M.} and Foucher, {Alexandre C.} and Stach, {Eric A.} and Sichao Ma and Kuhl, {Kendra P.} and Juergen Biener",

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Qi, Z, Kashi, AR, Buckley, AK, Miller, JS, Ye, J, Biener, MM, Foucher, AC, Stach, EA, Ma, S, Kuhl, KP & Biener, J 2022, 'Effect of Gold Catalyst Surface Morphology on Wetting Behavior and Electrochemical CO₂Reduction Performance in a Large-Area Zero-Gap Gas Diffusion Electrolyzer', Journal of Physical Chemistry C, vol. 126, no. 46, pp. 19637-19646. https://doi.org/10.1021/acs.jpcc.2c03773

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AU - Kuhl, Kendra P.

AU - Biener, Juergen

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