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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]
  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 Lab. (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. https://doi.org/10.1149/2.0181609jes.
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
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.
@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 = {2016},
month = {1}
}

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