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Title: Cerium migration during PEM fuel cell accelerated stress testing

Abstract

Cerium is a radical scavenger which improves polymer electrolyte membrane (PEM) fuel cell durability. During operation, however, cerium rapidly migrates in the PEM and into the catalyst layers (CLs). In this work, membrane electrode assemblies (MEAs) were subjected to accelerated stress tests (ASTs) under different humidity conditions. Cerium migration was characterized in the MEAs after ASTs using X-ray fluorescence. During fully humidified operation, water flux from cell inlet to outlet generated in-plane cerium gradients. Conversely, cerium profiles were flat during low humidity operation, where in-plane water flux was negligible, however, migration from the PEM into the CLs was enhanced. Humidity cycling resulted in both in-plane cerium gradients due to water flux during the hydration component of the cycle, and significant migration into the CLs. Fluoride and cerium emissions into effluent cell waters were measured during ASTs and correlated, which signifies that ionomer degradation products serve as possible counter-ions for cerium emissions. Fluoride emission rates were also correlated to final PEM cerium contents, which indicates that PEM degradation and cerium migration are coupled. Lastly, it is proposed that cerium migrates from the PEM due to humidification conditions and degradation, and is subsequently stabilized in the CLs by carbon catalyst supports.

Authors:
 [1];  [2];  [2];  [2];  [2];  [3];  [3]
+ Show Author Affiliations
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of Delaware, Newark, DE (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  3. Univ. of Delaware, Newark, DE (United States)
Publication Date:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE). Fuel Cell Technologies Program (EE-3F)
OSTI Identifier:
1291233
Report Number(s):
LA-UR-16-22054
Journal ID: ISSN 0013-4651
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 163; Journal Issue: 9; Journal ID: ISSN 0013-4651
Country of Publication:
United States
Language:
English
Subject:
30 DIRECT ENERGY CONVERSION; 36 MATERIALS SCIENCE; Energy Sciences; PEM, fuel cell, cerium, migration, performance, durability

Citation Formats

Baker, Andrew M., Mukundan, Rangachary, Borup, Rodney L., Spernjak, Dusan, Judge, Elizabeth J., Advani, Suresh G., and Prasad, Ajay K. Cerium migration during PEM fuel cell accelerated stress testing. United States: N. p., 2016. Web. doi:10.1149/2.0181609jes.
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Baker, Andrew M., Mukundan, Rangachary, Borup, Rodney L., Spernjak, Dusan, Judge, Elizabeth J., Advani, Suresh G., & Prasad, Ajay K. Cerium migration during PEM fuel cell accelerated stress testing. United States. https://doi.org/10.1149/2.0181609jes
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Baker, Andrew M., Mukundan, Rangachary, Borup, Rodney L., Spernjak, Dusan, Judge, Elizabeth J., Advani, Suresh G., and Prasad, Ajay K. Fri . "Cerium migration during PEM fuel cell accelerated stress testing". United States. https://doi.org/10.1149/2.0181609jes. https://www.osti.gov/servlets/purl/1291233.
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@article{osti_1291233,
title = {Cerium migration during PEM fuel cell accelerated stress testing},
author = {Baker, Andrew M. and Mukundan, Rangachary and Borup, Rodney L. and Spernjak, Dusan and Judge, Elizabeth J. and Advani, Suresh G. and Prasad, Ajay K.},
abstractNote = {Cerium is a radical scavenger which improves polymer electrolyte membrane (PEM) fuel cell durability. During operation, however, cerium rapidly migrates in the PEM and into the catalyst layers (CLs). In this work, membrane electrode assemblies (MEAs) were subjected to accelerated stress tests (ASTs) under different humidity conditions. Cerium migration was characterized in the MEAs after ASTs using X-ray fluorescence. During fully humidified operation, water flux from cell inlet to outlet generated in-plane cerium gradients. Conversely, cerium profiles were flat during low humidity operation, where in-plane water flux was negligible, however, migration from the PEM into the CLs was enhanced. Humidity cycling resulted in both in-plane cerium gradients due to water flux during the hydration component of the cycle, and significant migration into the CLs. Fluoride and cerium emissions into effluent cell waters were measured during ASTs and correlated, which signifies that ionomer degradation products serve as possible counter-ions for cerium emissions. Fluoride emission rates were also correlated to final PEM cerium contents, which indicates that PEM degradation and cerium migration are coupled. Lastly, it is proposed that cerium migrates from the PEM due to humidification conditions and degradation, and is subsequently stabilized in the CLs by carbon catalyst supports.},
doi = {10.1149/2.0181609jes},
journal = {Journal of the Electrochemical Society},
number = 9,
volume = 163,
place = {United States},
year = {Fri Jan 01 00:00:00 EST 2016},
month = {Fri Jan 01 00:00:00 EST 2016}
}
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Publisher's Version of Record
https://doi.org/10.1149/2.0181609jes
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Works referencing / citing this record:

Membrane Accelerated Stress Test Development for Polymer Electrolyte Fuel Cell Durability Validated Using Field and Drive Cycle Testing
journal, January 2018

  • Mukundan, Rangachary; Baker, Andrew M.; Kusoglu, Ahmet
  • Journal of The Electrochemical Society, Vol. 165, Issue 6
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Durability of Newly Developed Polyphenylene-Based Ionomer Membranes in Polymer Electrolyte Fuel Cells: Accelerated Stress Evaluation
journal, January 2019

  • Shimizu, Ryo; Otsuji, Kanji; Masuda, Akihiro
  • Journal of The Electrochemical Society, Vol. 166, Issue 7
  • DOI: 10.1149/2.0131907jes

Electrode Edge Cobalt Cation Migration in an Operating Fuel Cell: An In Situ Micro-X-ray Fluorescence Study
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  • Cai, Yun; Ziegelbauer, Joseph M.; Baker, Andrew M.
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Accelerated Stress Testing of Fuel Cell Membranes Subjected to Combined Mechanical/Chemical Stressors and Cerium Migration
journal, January 2018

  • Lai, Yeh-Hung; Rahmoeller, Kenneth M.; Hurst, James H.
  • Journal of The Electrochemical Society, Vol. 165, Issue 6
  • DOI: 10.1149/2.0241806jes

Predicting Membrane Lifetime with Cerium Oxide in Heavy Duty Fuel Cell Systems
journal, January 2018

  • Macauley, Natalia; Lauritzen, Michael; Knights, Shanna
  • Journal of The Electrochemical Society, Vol. 165, Issue 10
  • DOI: 10.1149/2.0271810jes

Migration of Ce and Mn Ions in PEMFC and Its Impact on PFSA Membrane Degradation
journal, January 2018

  • Zatoń, Marta; Prélot, Benedicte; Donzel, Nicolas
  • Journal of The Electrochemical Society, Vol. 165, Issue 6
  • DOI: 10.1149/2.0311806jes

CO 2 -Assisted Regeneration of a Polymer Electrolyte Water Electrolyzer Contaminated with Metal Ion Impurities
journal, January 2019

  • Babic, Ugljesa; Zlobinski, Mateusz; Schmidt, Thomas Justus
  • Journal of The Electrochemical Society, Vol. 166, Issue 10
  • DOI: 10.1149/2.0851910jes

Chemical Stability via Radical Decomposition Using Silicotungstic Acid Moieties for Polymer Electrolyte Fuel Cells
journal, January 2018

  • Motz, Andrew R.; Kuo, Mei-Chen; Bender, Guido
  • Journal of The Electrochemical Society, Vol. 165, Issue 14
  • DOI: 10.1149/2.1361814jes

CO2-assisted regeneration of a polymer electrolyte water electrolyzer contaminated with metal ion impurities
text, January 2019

Durability of Newly Developed Polyphenylene-Based Ionomer Membranes in Polymer Electrolyte Fuel Cells: Accelerated Stress Evaluation
journal, September 2019

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