Comparison of Different Carbon Supports By Simulation of Agglomeration in Polymer Electrolyte Fuel Cell Catalyst Ink
Authors: Saito Yuki , So Magnus , Inoue Gen 
Published: February 2024

Polymer electrolyte fuel cells (PEFCs) are one of the most possible power sources for heavy-duty vehicles like trucks due to their high conversion efficiency and low environmental impact. Since platinum which is often used as a catalyst is expensive, it is essential to reduce the amount of platinum by increasing the power density. Regarding materials, it was reported that the activity is increased by supporting platinum on porous carbon [1]. However, there is a voltage drop in the high current density region comparing non-porous carbon. This is caused by oxygen transport properties, but the relationship with the carbon structure is unknown. Oxygen moves through the voids in the catalyst layer, so it is necessary to control the porous structure that forms the voids. This porous structure depends on the conditions of the catalyst layer fabrication process. In particular, the dispersion process is important to determine the size of the carbon agglomerate, or the backbone of the catalyst layer. In this study, an agglomeration model in catalyst ink was developed, and the dispersion process was verified by simulation under various conditions to elucidate the factors that affect agglomeration.
The discrete element method (DEM) was used for the simulation. In this study, aggregates were approximated into spheres, and the forces between the particles were the drag force from the fluid, Brownian motion, and particle-particle interactions. Based on DLVO theory, the particle-particle interactions were given as an attractive force due to the van der Waals interaction and a repulsive force due to the overlapping of the electric double layer. In addition, the effect of ionomer was considered. The ionomer effect was introduced as a repulsive force and modeled with the same equation as the repulsion due to the electric double layer. The dielectric dependence equation of the ionomer shape that Magnus et al. modeled [2] was incorporated. As the amount of ionomer added increases, a binder effect is observed between the particles. This effect was also introduced using the adsorption data of ionomers on carbon. The carbon was assumed to be non-porous (Vulcan) and porous (Ketjen). Considering the difference in the platinum ratio on the surface depending on the carbon porosity, the Hamaker constant, which affects the van der Waals force, was determined. Also, the zeta potential, which affects the electric double layer force, was used at different values for carbons. In this study, the calculations were started with the particles uniformly dispersed in the ink. Periodic boundary conditions were used as boundary conditions. Using the above numerical model, simulations were conducted with different water-alcohol ratios and ionomer carbon ratios (I/C).
As a result, it was confirmed that differences in the agglomerate size for two carbon supports. This result implies that the composition of the ink and the type of carbon affect the catalyst layer structure and cell performance.
Acknowledgment
This study was carried out under the project of Development of Advanced PEFC Utilization Technologies supported by the NEDO.
Reference
[1] Y. C. Park et al., J. Pow. Sou
r., 315, 179 (2016).
[2] M. So et al., Int. J. Hydrog. Energy, 44, 28984 (2019).