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Title: Durability of De-Alloyed Platinum-Nickel Cathode Catalyst in Low Platinum Loading Membrane-Electrode Assemblies Subjected to Accelerated Stress Tests

Abstract

Here, the durability of de-alloyed platinum-nickel catalysts supported on high-surface area carbon (d-PtNi/C) in optimized electrodes and membrane electrode assemblies (MEAs) under an accelerated stress test (AST) protocol is investigated with the objective of developing a quantitative understanding of the degradation mechanisms and their relationship to the electrode structure, pre-conditioning, and operating conditions. It is found that the cell degradation can be mitigated by controlling the voltage cycle, acid washing the MEA to remove Ni contaminants that enter the electrode and membrane during fabrication, and monitoring the operating conditions. For example, the electrochemical surface area (ECSA) loss is <25% after 30,000 triangle cycles with 0.925 V upper potential limit if the MEA is acid washed and extensive diagnostics are avoided. The parameters that exacerbate the cell degradation also accelerate the rate at which Ni leaches out from the catalyst. A mechanistic model is presented for the degradation in performance of d-PtNi/C electrodes. The model correlates a) the degradation in ORR mass and specific activities with ECSA and Ni losses, b) the decrease in limiting current density ( iL), which is inversely proportional to the O 2 mass transport resistance, with the degradation in catalyst roughness factor, and c) the increasemore » in mass transfer overpotentials with the reduced current density, i/iL .« less

Authors:
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)
OSTI Identifier:
1434558
Alternate Identifier(s):
OSTI ID: 1437277
Grant/Contract Number:  
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: 165 Journal Issue: 6; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Catalyst durability; Mass transfer in cathode catalysts; Polymer electrolyte fuel cells

Citation Formats

Ahluwalia, R. K., Wang, X., Peng, J-K, Kariuki, N. N., Myers, D. J., Rasouli, S., Ferreira, P. J., Yang, Z., Martinez-Bonastre, A., Fongalland, D., and Sharman, J. Durability of De-Alloyed Platinum-Nickel Cathode Catalyst in Low Platinum Loading Membrane-Electrode Assemblies Subjected to Accelerated Stress Tests. United States: N. p., 2018. Web. doi:10.1149/2.0341806jes.
Ahluwalia, R. K., Wang, X., Peng, J-K, Kariuki, N. N., Myers, D. J., Rasouli, S., Ferreira, P. J., Yang, Z., Martinez-Bonastre, A., Fongalland, D., & Sharman, J. Durability of De-Alloyed Platinum-Nickel Cathode Catalyst in Low Platinum Loading Membrane-Electrode Assemblies Subjected to Accelerated Stress Tests. United States. doi:10.1149/2.0341806jes.
Ahluwalia, R. K., Wang, X., Peng, J-K, Kariuki, N. N., Myers, D. J., Rasouli, S., Ferreira, P. J., Yang, Z., Martinez-Bonastre, A., Fongalland, D., and Sharman, J. Fri . "Durability of De-Alloyed Platinum-Nickel Cathode Catalyst in Low Platinum Loading Membrane-Electrode Assemblies Subjected to Accelerated Stress Tests". United States. doi:10.1149/2.0341806jes.
@article{osti_1434558,
title = {Durability of De-Alloyed Platinum-Nickel Cathode Catalyst in Low Platinum Loading Membrane-Electrode Assemblies Subjected to Accelerated Stress Tests},
author = {Ahluwalia, R. K. and Wang, X. and Peng, J-K and Kariuki, N. N. and Myers, D. J. and Rasouli, S. and Ferreira, P. J. and Yang, Z. and Martinez-Bonastre, A. and Fongalland, D. and Sharman, J.},
abstractNote = {Here, the durability of de-alloyed platinum-nickel catalysts supported on high-surface area carbon (d-PtNi/C) in optimized electrodes and membrane electrode assemblies (MEAs) under an accelerated stress test (AST) protocol is investigated with the objective of developing a quantitative understanding of the degradation mechanisms and their relationship to the electrode structure, pre-conditioning, and operating conditions. It is found that the cell degradation can be mitigated by controlling the voltage cycle, acid washing the MEA to remove Ni contaminants that enter the electrode and membrane during fabrication, and monitoring the operating conditions. For example, the electrochemical surface area (ECSA) loss is <25% after 30,000 triangle cycles with 0.925 V upper potential limit if the MEA is acid washed and extensive diagnostics are avoided. The parameters that exacerbate the cell degradation also accelerate the rate at which Ni leaches out from the catalyst. A mechanistic model is presented for the degradation in performance of d-PtNi/C electrodes. The model correlates a) the degradation in ORR mass and specific activities with ECSA and Ni losses, b) the decrease in limiting current density (iL), which is inversely proportional to the O2 mass transport resistance, with the degradation in catalyst roughness factor, and c) the increase in mass transfer overpotentials with the reduced current density, i/iL .},
doi = {10.1149/2.0341806jes},
journal = {Journal of the Electrochemical Society},
number = 6,
volume = 165,
place = {United States},
year = {2018},
month = {3}
}

Journal Article:
Free Publicly Available Full Text
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DOI: 10.1149/2.0341806jes

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