Modeling the Morphological Effects of Catalyst and Ionomer Loading on Porous Carbon Supports of PEMFC

We present a model of the cathode catalyst layer morphology before and after loading a porous catalyst support with Pt and ionomer. Support nanopores and catalyst particles within pores and on the support surface are described by size distributions, allowing for qualitative processes during the addition of a material phase to be dependent on the observed pore and particle size. A particular focus is put on the interplay of pore impregnation and blockage due to ionomer loading and the consequences for the Pt/ionomer interface, ionomer film thickness and protonic binding of particles within pores. We used the model to emulate six catalyst/support combinations from literature with different porosity, surface area and pore size distributions of the support as well as varying particle size distributions and ionomer/carbon ratios. Besides providing qualitatively and quantitatively accurate predictions, the model is able to explain why the protonically active catalyst surface area has been reported to not increase monotonically with ionomer addition for some supports, but rather decrease again when the optimum ionomer content is exceeded. The proposed model constitutes a fast translation from manufacturing parameters to catalyst layer morphology which can be incorporated into existing performance and degradation models in a straightforward way.

Automated summary

We propose a model that can simulate the morphology of the cathode catalyst layer before and after loading with Pt and ionomer. The model accurately describes the size distributions of support nanopores and catalyst particles, allowing for qualitative predictions during the addition of materials. The model focuses on the impregnation and blockage of pores due to ionomer loading and its consequences on the Pt/ionomer interface, ionomer film thickness, and protonic binding. It successfully emulates different catalyst/support combinations and explains the non-monotonic increase of protonically active catalyst surface area with ionomer addition in some supports.