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A PEM fuel cell with a hydrophobically treated cathode catalyst layer (CL) demonstrates ∼220% peak power increase with humidified air at 70 °C. To understand the reasons of the increase, a mathematical model was developed focusing on the oxygen-water two-phase transport phenomena in the CL. It suggests the treatment affects the CL in two ways. First, the interface of the ionomer layer exposed to the gas pores becomes more hydrophobic, facilitating less liquid water coverage and faster water drainage from the CL and resulting in better performance at high current densities. Second, it also affects the hydration level in the ionomer phase resulting in higher oxygen concentration in the ionomer phase on and in the catalyst agglomerates, leading to higher performance over the whole polarization curve. The properties having significant influence on the model fitting the experimental data are the capillary pressure property of the CL, the hydrophobic ionomer ratio in the catalyst agglomerate, and the oxygen solubility/diffusivity in the Nafion® phases. With this experimentally verified model, additional case studies combining the hydrophobic gas diffusion material with the hydrophobic CL demonstrate that the membrane’s self-humidification (zero-net-water flux) and peak power enhancement (∼15%) can be reached simultaneously, providing direction for the future materials development. 

During high current density operation, water production in the polymer electrolyte membrane fuel cell (PEMFC) cathode catalyst layer can negatively affect performance by lowering mass transport of oxygen into the cathode. In this paper, a novel heat treatment process for controlling the ionic polymer/gas interface property of the fuel cell catalyst layer is investigated and then incorporated into the membrane electrode assembly (MEA) fabrication process. XPS characterization of the catalyst layer’s ionomer-gas interface at its outer surface and its sublayers’ surfaces obtained by scraping off successive layers of the catalyst layers confirms that a hydrophobic ionomer interface can be achieved across the catalyst layer using a specific heat treatment condition. Based on the results of the catalyst layer study, the MEA fabrication process is modified to identify heat treatment configuration and conditions that will create an optimal hydrophobic ionomer-gas interface inside the cathode catalyst layer. Finally, fuel cell tests conducted on the conventional and new MEAs under different operating temperatures show the performance of the fuel cells with the treated MEAs was > 130% higher than that with the conventional MEA at 25 °C and 70 °C with humidified air and > 45% higher at 70 °C with dry air. The durability of the hydrophobic treatment on the cathode catalyst layer ionomer is also confirmed by the accelerated stress test.