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Title: Long-term stability of nanostructured thin film electrodes at operating potentials

Abstract

Long-term stability of nanostructured thin film (NSTF) catalysts at operating potentials has been investigated. Compared to high surface area Pt/C catalysts, NSTF electrodes show 20–50x smaller F emission rates (FER) because of their high specific activity for oxygen reduction reaction (ORR), but are susceptible to poisoning by the products of membrane degradation because of their low electrochemically active surface area (ECSA). The observed voltage degradation rates at potentials corresponding to 1–1.5 A/cm 2 current density are much higher than the allowable 13–14 μV/h. Although F is not itself responsible for performance decay, cumulative fluoride release (CFR) is a good marker for catalyst surface contamination. The observed performance decay is not only due to loss of active Pt sites but also adsorbed impurities impeding ORR kinetics. There is a strong correlation between measured CFR and observed decrease in specific ORR activity and limiting current density and increase in mass transfer overpotentials. Furthermore, the correlations indicate that the target of <10% lifetime performance degradation can be achieved by restricting CFR in NSTF electrodes to 0.7 μg/cm 2, as may be possible with more stable membranes, higher surface area NSTF catalysts, and cell operation at lower temperatures and higher relative humidities.

Authors:
 [1];  [1];  [1];  [2];  [3]
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. 3M Fuel Cell Components Program, St. Paul, MN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Fuel Cell Technologies Office (EE-3F)
OSTI Identifier:
1345010
Alternate Identifier(s):
OSTI ID: 1373711
Grant/Contract Number:
AC05-00OR22725; AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 164; Journal Issue: 4; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; mass transfer in cathode catalysts; nanostructured thin film electrodes; oxygen reduction reaction kinetics; polymer electrolyte fuel cells; stability and durability

Citation Formats

Ahluwalia, Rajesh K., Peng, J. -K., Wang, X., Cullen, David A., and Steinbach, Andrew J. Long-term stability of nanostructured thin film electrodes at operating potentials. United States: N. p., 2017. Web. doi:10.1149/2.0881704jes.
Ahluwalia, Rajesh K., Peng, J. -K., Wang, X., Cullen, David A., & Steinbach, Andrew J. Long-term stability of nanostructured thin film electrodes at operating potentials. United States. doi:10.1149/2.0881704jes.
Ahluwalia, Rajesh K., Peng, J. -K., Wang, X., Cullen, David A., and Steinbach, Andrew J. Thu . "Long-term stability of nanostructured thin film electrodes at operating potentials". United States. doi:10.1149/2.0881704jes. https://www.osti.gov/servlets/purl/1345010.
@article{osti_1345010,
title = {Long-term stability of nanostructured thin film electrodes at operating potentials},
author = {Ahluwalia, Rajesh K. and Peng, J. -K. and Wang, X. and Cullen, David A. and Steinbach, Andrew J.},
abstractNote = {Long-term stability of nanostructured thin film (NSTF) catalysts at operating potentials has been investigated. Compared to high surface area Pt/C catalysts, NSTF electrodes show 20–50x smaller F– emission rates (FER) because of their high specific activity for oxygen reduction reaction (ORR), but are susceptible to poisoning by the products of membrane degradation because of their low electrochemically active surface area (ECSA). The observed voltage degradation rates at potentials corresponding to 1–1.5 A/cm2 current density are much higher than the allowable 13–14 μV/h. Although F– is not itself responsible for performance decay, cumulative fluoride release (CFR) is a good marker for catalyst surface contamination. The observed performance decay is not only due to loss of active Pt sites but also adsorbed impurities impeding ORR kinetics. There is a strong correlation between measured CFR and observed decrease in specific ORR activity and limiting current density and increase in mass transfer overpotentials. Furthermore, the correlations indicate that the target of <10% lifetime performance degradation can be achieved by restricting CFR in NSTF electrodes to 0.7 μg/cm2, as may be possible with more stable membranes, higher surface area NSTF catalysts, and cell operation at lower temperatures and higher relative humidities.},
doi = {10.1149/2.0881704jes},
journal = {Journal of the Electrochemical Society},
number = 4,
volume = 164,
place = {United States},
year = {Thu Feb 09 00:00:00 EST 2017},
month = {Thu Feb 09 00:00:00 EST 2017}
}

Journal Article:
Free Publicly Available Full Text
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