Zoom in Catalyst/Ionomer Interface in Polymer Electrolyte Membrane Fuel Cell Electrodes: Impact of Catalyst/Ionomer Dispersion Media/Solvent

Large-scale applications of polymer electrolyte membrane fuel cells (PEMFCs) are throttled primarily by high initial cost and durability issues of the electrodes, which essentially consist of the nanoparticulate catalysts (e.g., Pt) having accessibility to electrons (e–), protons (H+), and fuel/oxidant through catalyst support, polymer electrolyte ionomer, and porous gas diffusion layer, respectively. Hence, to achieve high electrode performance in terms of activity and/or durability, understanding and optimization of the catalyst/support and catalyst/ionomer interfaces are of significant importance. Present study demonstrates an alternative route to inspect the catalyst/ionomer interface through an accelerated stress test combined with electrochemical impedance spectroscopy. Various interfaces are created through catalyst inks prepared using commercial Pt/C catalyst powder dispersed in different solvents. Electrode degradation pattern turns out to be a very useful tool to interpret a catalyst/ionomer interface structure. Variations of interfacial impedance, electrochemical surface area (ECSA), and double layer capacitance with the number of potential cycles suggested significant impact of catalyst/ionomer interface on the catalyst performance. A quantification of the degradation mechanisms responsible for ECSA loss during AST was employed to further understand the correlations between the electrochemical performance of the electrodes and their catalyst/ionomer interface structures. The knowledge may be implied to further optimize the electrode structure and hence to advance the PEMFC technology.