In-Situ Modeling of Chemical Membrane Degradation and Mitigation in Ceria-Supported Fuel Cells

Ceria-supported membrane electrode assemblies (MEAs) have recently been proposed to address chemical membrane degradation in polymer electrolyte fuel cells. Although ceria is known to effectively protect the membrane at open circuit voltage (OCV) conditions, its effectiveness has not been demonstrated for cell voltages below OCV and associated conditions relevant for field operation. In the present work, a comprehensive, transient in situ chemical degradation model for ceria stabilized MEAs is developed and applied to investigate the mitigation effectiveness of ceria additive. At high cell voltages, abundant Ce3+ ions are available in the membrane to quench hydroxyl radicals which is the primary mitigation mechanism observed at OCV conditions. However, the mitigation is suppressed at low cell voltages, where electromigration drives Ce3+ ions into the cathode catalyst layer (CL). Without an adequate amount of Ce3+ in the membrane, the hydroxyl radical scavenging is significantly reduced, leading to a ten-fold reduction in mitigation effectiveness at cell voltages below 0.7 V. The simulated results also suggest that significant ceria precipitation may occur in the cathode CL due to the increased local Ce3+ concentration at low to medium cell voltages. Ceria-supported MEAs may therefore experience higher rates of chemical membrane degradation at low cell voltages than at OCV. (C) The Author(s) 2017. Published by ECS. All rights reserved.