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Title: Zr-doped ceria additives for enhanced PEM fuel cell durability and radical scavenger stability

Doped ceria compounds demonstrate excellent radical scavenging abilities and are promising additives to improve the chemical durability of polymer electrolyte membrane (PEM) fuel cells. Here in this paper, Ce 0.85Zr 0.15O 2 (CZO) nanoparticles were incorporated into the cathode catalyst layers (CLs) of PEM fuel cells (based on Nafion XL membranes containing 6.0 μg cm -2 ion-exchanged Ce) at loadings of 10 and 55 μg cm -2. When compared to a CZO-free baseline, CZO-containing membrane electrode assemblies (MEAs) demonstrated extended lifetimes during PEM chemical stability accelerated stress tests (ASTs), exhibiting reduced electrochemical gas crossover, open circuit voltage decay, and fluoride emission rates. The MEA with high CZO loading (55 μg cm -2) demonstrated performance losses, which are attributed to Ce poisoning of the PEM and CL ionomer regions, which is supported by X-ray fluorescence (XRF) analysis. In the MEA with the low CZO loading (10 μg cm -2), both the beginning of life (BOL) performance and the performance after 500 hours of ASTs were nearly identical to the BOL performance of the CZO-free baseline MEA. XRF analysis of the MEA with low CZO loading reveals that the BOL PEM Ce concentrations are preserved after 1408 hours of ASTs and thatmore » Ce contents in the cathode CL are not significant enough to reduce performance. Therefore, employing a highly effective radical scavenger such as CZO, at a loading of 10 μg cm -2 in the cathode CL, dramatically mitigates degradation effects, which improves MEA chemical durability and minimizes performance losses.« less
Authors:
ORCiD logo [1] ;  [2] ; ORCiD logo [2] ; ORCiD logo [2] ;  [3] ;  [3] ; ORCiD logo [2]
  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:
Report Number(s):
LA-UR-17-23340
Journal ID: ISSN 2050-7488; TRN: US1703160
Grant/Contract Number:
AC52-06NA25396
Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 5; Journal Issue: 29; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
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)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Energy Sciences
OSTI Identifier:
1407888

Baker, Andrew M., Williams, Stefan Thurston DuBard, Mukundan, Rangachary, Spernjak, Dusan, Advani, Suresh G., Prasad, Ajay K., and Borup, Rodney L.. Zr-doped ceria additives for enhanced PEM fuel cell durability and radical scavenger stability. United States: N. p., Web. doi:10.1039/C7TA03452K.
Baker, Andrew M., Williams, Stefan Thurston DuBard, Mukundan, Rangachary, Spernjak, Dusan, Advani, Suresh G., Prasad, Ajay K., & Borup, Rodney L.. Zr-doped ceria additives for enhanced PEM fuel cell durability and radical scavenger stability. United States. doi:10.1039/C7TA03452K.
Baker, Andrew M., Williams, Stefan Thurston DuBard, Mukundan, Rangachary, Spernjak, Dusan, Advani, Suresh G., Prasad, Ajay K., and Borup, Rodney L.. 2017. "Zr-doped ceria additives for enhanced PEM fuel cell durability and radical scavenger stability". United States. doi:10.1039/C7TA03452K. https://www.osti.gov/servlets/purl/1407888.
@article{osti_1407888,
title = {Zr-doped ceria additives for enhanced PEM fuel cell durability and radical scavenger stability},
author = {Baker, Andrew M. and Williams, Stefan Thurston DuBard and Mukundan, Rangachary and Spernjak, Dusan and Advani, Suresh G. and Prasad, Ajay K. and Borup, Rodney L.},
abstractNote = {Doped ceria compounds demonstrate excellent radical scavenging abilities and are promising additives to improve the chemical durability of polymer electrolyte membrane (PEM) fuel cells. Here in this paper, Ce0.85Zr0.15O2 (CZO) nanoparticles were incorporated into the cathode catalyst layers (CLs) of PEM fuel cells (based on Nafion XL membranes containing 6.0 μg cm-2 ion-exchanged Ce) at loadings of 10 and 55 μg cm-2. When compared to a CZO-free baseline, CZO-containing membrane electrode assemblies (MEAs) demonstrated extended lifetimes during PEM chemical stability accelerated stress tests (ASTs), exhibiting reduced electrochemical gas crossover, open circuit voltage decay, and fluoride emission rates. The MEA with high CZO loading (55 μg cm-2) demonstrated performance losses, which are attributed to Ce poisoning of the PEM and CL ionomer regions, which is supported by X-ray fluorescence (XRF) analysis. In the MEA with the low CZO loading (10 μg cm-2), both the beginning of life (BOL) performance and the performance after 500 hours of ASTs were nearly identical to the BOL performance of the CZO-free baseline MEA. XRF analysis of the MEA with low CZO loading reveals that the BOL PEM Ce concentrations are preserved after 1408 hours of ASTs and that Ce contents in the cathode CL are not significant enough to reduce performance. Therefore, employing a highly effective radical scavenger such as CZO, at a loading of 10 μg cm-2 in the cathode CL, dramatically mitigates degradation effects, which improves MEA chemical durability and minimizes performance losses.},
doi = {10.1039/C7TA03452K},
journal = {Journal of Materials Chemistry. A},
number = 29,
volume = 5,
place = {United States},
year = {2017},
month = {6}
}