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Gas diffusion layers (GDLs) play a crucial role in heat transfer and water management of cathode catalyst layers in polymer electrolyte fuel cells (PEFCs). Thermal and water gradients can accelerate electrocatalyst degradation and therefore the selection of GDLs can have a major influence on PEFC durability. Currently, the role of GDLs in electrocatalyst degradation is poorly studied. Here, we perform electrocatalyst accelerated stress test studies on membrane electrode assemblies (MEAs) prepared using three most commonly used GDLs. The effect of GDLs on electrocatalyst degradation is evaluated in both nitrogen (non-reactive) and air (reactive) gas environments at 100% relative humidity. Inmore » situ electrochemical characterization and extensive physical characterization is performed to understand the subtle differences in electrocatalyst degradation and correlated to the use of different GDLs. Overall, no difference is observed in the electrocatalyst degradation due to GDLs based on polarization curves at the end of life. But interestingly, MEA with a cracked microporous layer (MPL) in the GDL exhibited a higher electrocatalyst loading loss, which resulted in a lower and more heterogeneous increase in the average electrocatalyst nanoparticle size.« less

Batteries capable of extreme fast-charging (XFC) are a necessity for the deployment of electric vehicles. Material properties of electrodes and electrolytes along with cell parameters such as stack pressure and temperature have coupled, synergistic, and sometimes deleterious effects on fast-charging performance. We develop a new experimental testbed that allows precise and conformal application of electrode stack pressure. We focus on cell capacity degradation using single-layer pouch cells with graphite anodes, LiNi0.5Mn0.3Co0.2O2 (NMC532) cathodes, and carbonate-based electrolyte. In the tested range (10–125 psi), cells cycled at higher pressure show higher capacity and less capacity fading. Additionally, Li plating decreases with increasingmore » pressure as observed with scanning electron microscopy (SEM) and optical imaging. While the loss of Li inventory from Li plating is the largest contributor to capacity fade, electrochemical and SEM examination of the NMC cathodes after XFC experiments show increased secondary particle damage at lower pressure. We infer that the better performance at higher pressure is due to more homogeneous reactions of active materials across the electrode and less polarization through the electrode thickness. Our study emphasizes the importance of electrode stack pressure in XFC batteries and highlights its subtle role in cell conditions.« less

The heterogeneity of polymer electrolyte fuel cell catalyst degradation is studied under varied relative humidity and types of feed gas. Accelerated stress tests (ASTs) are performed on four membrane electrode assemblies (MEAs) under wet and dry conditions in an air or nitrogen environment for 30 000 square voltage cycles. The largest electrochemically active area loss is observed for MEA under wet conditions in a nitrogen gas environment AST due to constant upper potential limit of 0.95 V and significant water content. The mean Pt particle size is larger for the ASTs under wet conditions compared to dry conditions, and the Ptmore » particle size under land is generally larger than under the channel. Observations from ASTs in both conditions and gas environments indicate that water content promotes Pt particle size growth. ASTs under wet conditions and an air environment show the largest difference in Pt particle size growth for inlet versus outlet and channel versus land, which can be attributed to larger water content at outlet and under land compared to inlet and under channel. From X-ray fluorescence experiments Pt particle size increase is a local phenomenon as Pt loading remains relatively uniform across the MEA.« less

Pt catalysts in polymer electrolyte fuel cells degrade heterogeneously as the catalyst particles are exposed to local variations throughout the catalyst layer during operation. State-of-the-art analytical techniques for studying degradation of Pt catalysts do not possess fine spatial resolution to elucidate such non-uniform degradation behavior at a large electrode level. A new methodology is developed to spatially resolve and quantify the heterogeneous Pt catalyst degradation over a large area (several cm ) of aged MEAs based on synchrotron X-ray microdiffraction. PEFC single cells are aged using voltage cycling as an accelerated stress test and the degradation heterogeneity at a micrometermore » length scale is visualized by mapping Pt catalyst particle size after voltage cycling. It is demonstrated in detail that the Pt catalyst particle size growth is non-uniform and follows the flow field geometry. The Pt particle size growth is greater in the area under the flow field land, while it is minimal in the area under the flow field channel. Additional non-uniformity is observed with the Pt particle size increasing more rapidly at the air outlet area than the Pt particle size at the inlet area.« less