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Title: Durability of Polymer Electrolyte Membrane Fuel Cells Operated at Subfreezing Temperatures

The structure, composition, and interfaces of membrane electrode assemblies (MEA) and gas-diffusion layers (GDLs) have a significant effect on the performance of single-proton-exchange-membrane (PEM) fuel cells operated isothermally at subfreezing temperatures. During isothermal constant-current operation at subfreezing temperatures, water forming at the cathode initially hydrates the membrane, then forms ice in the catalyst layer and/or GDL. This ice formation results in a gradual decay in voltage. High-frequency resistance initially decreases due to an increase in membrane water content and then increases over time as the contact resistance increases. The water/ice holding capacity of a fuel cell decreases with decreasing subfreezing temperature (-10°C vs. -20°C vs. -30°C) and increasing current density (0.02 A cm -2 vs. 0.04 A cm -2). Ice formation monitored using in-situ high-resolution neutron radiography indicated that the ice was concentrated near the cathode catalyst layer at low operating temperatures (≈-20°C) and high current densities (0.04 A cm -2). Significant ice formation was also observed in the GDLs at higher subfreezing temperatures (≈-10°C) and lower current densities (0.02 A cm -2). These results are in good agreement with the long-term durability observations that show more severe degradation at lower temperatures (-20°C and -30°C).
Authors:
 [1] ;  [1] ;  [1] ;  [2] ;  [2] ;  [3] ;  [1] ;  [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Center for Neutron Research
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Report Number(s):
LA-UR-17-22338
Journal ID: ISSN 0013-4651
Grant/Contract Number:
AI01-01EE50660
Type:
Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 163; Journal Issue: 13; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Research Org:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States); National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Fuel Cell Technologies Office (EE-3F); Dept. of Commerce (United States)
Country of Publication:
United States
Language:
English
Subject:
30 DIRECT ENERGY CONVERSION; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; PEM fuel cell; electrolyzers; energy conversion; durability; subfreezing operation
OSTI Identifier:
1374332

Macauley, Natalia, Lujan, Roger W., Spernjak, Dusan, Hussey, Daniel S., Jacobson, David L., More, Karren, Borup, Rodney L., and Mukundan, Rangachary. Durability of Polymer Electrolyte Membrane Fuel Cells Operated at Subfreezing Temperatures. United States: N. p., Web. doi:10.1149/2.0191613jes.
Macauley, Natalia, Lujan, Roger W., Spernjak, Dusan, Hussey, Daniel S., Jacobson, David L., More, Karren, Borup, Rodney L., & Mukundan, Rangachary. Durability of Polymer Electrolyte Membrane Fuel Cells Operated at Subfreezing Temperatures. United States. doi:10.1149/2.0191613jes.
Macauley, Natalia, Lujan, Roger W., Spernjak, Dusan, Hussey, Daniel S., Jacobson, David L., More, Karren, Borup, Rodney L., and Mukundan, Rangachary. 2016. "Durability of Polymer Electrolyte Membrane Fuel Cells Operated at Subfreezing Temperatures". United States. doi:10.1149/2.0191613jes. https://www.osti.gov/servlets/purl/1374332.
@article{osti_1374332,
title = {Durability of Polymer Electrolyte Membrane Fuel Cells Operated at Subfreezing Temperatures},
author = {Macauley, Natalia and Lujan, Roger W. and Spernjak, Dusan and Hussey, Daniel S. and Jacobson, David L. and More, Karren and Borup, Rodney L. and Mukundan, Rangachary},
abstractNote = {The structure, composition, and interfaces of membrane electrode assemblies (MEA) and gas-diffusion layers (GDLs) have a significant effect on the performance of single-proton-exchange-membrane (PEM) fuel cells operated isothermally at subfreezing temperatures. During isothermal constant-current operation at subfreezing temperatures, water forming at the cathode initially hydrates the membrane, then forms ice in the catalyst layer and/or GDL. This ice formation results in a gradual decay in voltage. High-frequency resistance initially decreases due to an increase in membrane water content and then increases over time as the contact resistance increases. The water/ice holding capacity of a fuel cell decreases with decreasing subfreezing temperature (-10°C vs. -20°C vs. -30°C) and increasing current density (0.02 A cm-2 vs. 0.04 A cm-2). Ice formation monitored using in-situ high-resolution neutron radiography indicated that the ice was concentrated near the cathode catalyst layer at low operating temperatures (≈-20°C) and high current densities (0.04 A cm-2). Significant ice formation was also observed in the GDLs at higher subfreezing temperatures (≈-10°C) and lower current densities (0.02 A cm-2). These results are in good agreement with the long-term durability observations that show more severe degradation at lower temperatures (-20°C and -30°C).},
doi = {10.1149/2.0191613jes},
journal = {Journal of the Electrochemical Society},
number = 13,
volume = 163,
place = {United States},
year = {2016},
month = {9}
}