Improving the efficiency of polymer electrolyte fuel cells (PEFCs) through high power density operation necessitates liquid water management in the cathode gas diffusion layer (GDL), where liquid water saturation inhibits oxygen diffusivity. To this end, there have been numerous efforts aimed at understanding liquid water transport behaviour to guide GDL design improvements. X-ray imaging of representative in-operando miniaturized PEFC samples has been instrumental to much of recent progress [1–4] in understanding liquid water distribution patterns. Radiographic two-dimensional (2D) images have enabled visualization of liquid water dynamics [3] while three-dimensional (3D) computed tomography images have provided pore-scale information of liquid water saturation states in the GDL [2] and of its transport mechanism [4]. However, how liquid water pathways are formed and the likelihood for preferential pathways remain unclear.

In this work, we investigate factors that influence liquid water distribution and pathway definition using correlative rapid 2D and long duration 3D operando X-ray datasets which enable a visualization of liquid water breakthrough dynamics and the corresponding pore-scale interactions in the GDL. The correlated images together with GDL pore structure visualization are used to identify three characteristic pore-scale saturation behaviour with sample regions highlighted in Fig. 1. These regions include locations with restricted liquid water breakthrough, locations with apparent large breakthrough porous pathways where breakthrough liquid water is observable at least in the 2D images, and similarly porous regions where no liquid water breakthrough is observed. It is found that the behaviour shown in the identified regions are strongly linked to local pore-scale structural characteristics and capillary pressure distribution in the GDL. Investigating the 3D virtual GDL from around the microporous layer through to the channel interface, it is shown that liquid water pathways get increasingly defined with a decrease in spatial uniformity towards the flow channels. Pore-scale analysis and observed flow mechanisms show that the defined pathways are locally accessible paths of least capillary resistance dictated by pore radius and associated hydrophobicity. These findings highlight the important role that pore scale topology plays in addition to pore size distribution for future GDL design aimed at improving water management.

Keywords— operando, fuel cell, water, pore structure, X-ray imaging

Acknowledgments

Funding for this research was provided by the Natural Sciences and Engineering Research Council of Canada, Ballard Power Systems, Canada Foundation for Innovation, British Columbia Knowledge Development Fund, Western Economic Diversification Canada, and Canada Research Chairs.

References

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