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Title: Mitigation of PEM Fuel Cell Catalyst Degradation with Porous Carbon Supports

Abstract

Maintaining high performance after extensive use remains a key challenge for low-Pt proton exchange membrane fuel cells for transportation applications. Strategically improving catalyst durability requires better understanding of the relationship between degradation mechanisms and catalyst structure. To investigate the effects of the carbon support morphology, we compare the electrochemical performance and durability of membrane electrode assemblies (MEAs) using Pt and PtCox catalysts with a range of porous, solid, and intermediate carbon supports (HSC, Vulcan, and acetylene black). We find that electrochemical surface area (ECSA) retention after a catalyst-targeted durability test tends to improve with increasing support porosity. Using electron microscopy, we investigate microstructural changes in the catalysts and reveal the underlying degradation mechanisms in MEA specimens. Pt migration to the membrane and catalyst coarsening, measured microscopically, together were quantitatively consistent with the ECSA loss, indicating that these were the only two significant degradation pathways. Changes in catalyst particle size, morphology, and PtCo core-shell structure indicate that Ostwald ripening is a significant coarsening mechanism for catalysts on all carbons, while particle coalescence is only significant on the more solid carbon supports. Porous carbon supports thus appear to protect against particle coalescence, providing an effective strategy for mitigating catalyst coarsening.

Authors:
ORCiD logo; ORCiD logo; ; ; ; ; ; ; ; ORCiD logo;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Fuel Cell Technologies Office
OSTI Identifier:
1495620
Alternate Identifier(s):
OSTI ID: 1510484
Grant/Contract Number:  
EE0007271; AC02-06CH11357
Resource Type:
Published Article
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Name: Journal of the Electrochemical Society Journal Volume: 166 Journal Issue: 4; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Padgett, Elliot, Yarlagadda, Venkata, Holtz, Megan E., Ko, Matthew, Levin, Barnaby D. A., Kukreja, Ratandeep Singh, Ziegelbauer, Joseph M., Andrews, Ross N., Ilavsky, Jan, Kongkanand, Anusorn, and Muller, David A. Mitigation of PEM Fuel Cell Catalyst Degradation with Porous Carbon Supports. United States: N. p., 2019. Web. https://doi.org/10.1149/2.0371904jes.
Padgett, Elliot, Yarlagadda, Venkata, Holtz, Megan E., Ko, Matthew, Levin, Barnaby D. A., Kukreja, Ratandeep Singh, Ziegelbauer, Joseph M., Andrews, Ross N., Ilavsky, Jan, Kongkanand, Anusorn, & Muller, David A. Mitigation of PEM Fuel Cell Catalyst Degradation with Porous Carbon Supports. United States. https://doi.org/10.1149/2.0371904jes
Padgett, Elliot, Yarlagadda, Venkata, Holtz, Megan E., Ko, Matthew, Levin, Barnaby D. A., Kukreja, Ratandeep Singh, Ziegelbauer, Joseph M., Andrews, Ross N., Ilavsky, Jan, Kongkanand, Anusorn, and Muller, David A. Thu . "Mitigation of PEM Fuel Cell Catalyst Degradation with Porous Carbon Supports". United States. https://doi.org/10.1149/2.0371904jes.
@article{osti_1495620,
title = {Mitigation of PEM Fuel Cell Catalyst Degradation with Porous Carbon Supports},
author = {Padgett, Elliot and Yarlagadda, Venkata and Holtz, Megan E. and Ko, Matthew and Levin, Barnaby D. A. and Kukreja, Ratandeep Singh and Ziegelbauer, Joseph M. and Andrews, Ross N. and Ilavsky, Jan and Kongkanand, Anusorn and Muller, David A.},
abstractNote = {Maintaining high performance after extensive use remains a key challenge for low-Pt proton exchange membrane fuel cells for transportation applications. Strategically improving catalyst durability requires better understanding of the relationship between degradation mechanisms and catalyst structure. To investigate the effects of the carbon support morphology, we compare the electrochemical performance and durability of membrane electrode assemblies (MEAs) using Pt and PtCox catalysts with a range of porous, solid, and intermediate carbon supports (HSC, Vulcan, and acetylene black). We find that electrochemical surface area (ECSA) retention after a catalyst-targeted durability test tends to improve with increasing support porosity. Using electron microscopy, we investigate microstructural changes in the catalysts and reveal the underlying degradation mechanisms in MEA specimens. Pt migration to the membrane and catalyst coarsening, measured microscopically, together were quantitatively consistent with the ECSA loss, indicating that these were the only two significant degradation pathways. Changes in catalyst particle size, morphology, and PtCo core-shell structure indicate that Ostwald ripening is a significant coarsening mechanism for catalysts on all carbons, while particle coalescence is only significant on the more solid carbon supports. Porous carbon supports thus appear to protect against particle coalescence, providing an effective strategy for mitigating catalyst coarsening.},
doi = {10.1149/2.0371904jes},
journal = {Journal of the Electrochemical Society},
number = 4,
volume = 166,
place = {United States},
year = {2019},
month = {2}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1149/2.0371904jes

Citation Metrics:
Cited by: 10 works
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Figures / Tables:

Table I Table I: Physical properties of catalyst carbon supports.

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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.