Impact of the Drying Temperature during Catalyst Layer Manufacturing on PEM Fuel Cell Performance

The manufacturing process of catalyst coated membranes for polymer electrolyte fuel cells (PEMFC) needs to be transferred to high throughput mass production to meet the increasing demand on the market. After the coating of the catalyst ink, the drying temperature and its profile can change the pore structure and crack appearance of the catalyst layer by influencing the solvent evaporation [1]. Therefore, adjusting the drying parameters to the type of solvents within the catalyst ink can result in beneficial performance gain. Often solvents with low boiling points like isopropanol-water mixtures are used. The rapid evaporation of these solvents could lead to crack formation, which could be avoided by the usage of high boiling point solvents like e.g. ethylene glycol [2,3]. Therefore higher drying temperatures are necessary to ensure a complete removal of the wet components. This leads to the question of the maximum drying temperature which can be applied to speed up the drying process as much as possible. The most temperature sensitive component within the catalyst layer is the ionomer. Drying at high temperatures could lead to degradation and decomposition of the ionomer network within the catalyst layer. However, is the temperature too low, the necessary drying time increases, which would result in higher investment costs for longer drying process lines. Within this study we investigated at first the thermal behavior of short side chain (Aquivion®) and long side chain (Nafion™) ionomer dispersions to analyze their glass transition and melting temperatures with differential scanning calorimetry in the range of 30-400°C. The findings are shown in Figure 1. The glass transition temperature of Aquivion® lies between 154-159°C, whereas Nafion™ is more temperature sensitive with 125-142°C, which is consistent with the literature. In a second step, catalyst layers have been fabricated by screen printing with a catalyst paste including a solvent mixture of ethylene glycol and 1-methoxy-2-propanol [4]. The resulting catalyst layers have platinum loadings of 0.154 mg/cm² on the cathode and 0.05 mg/cm² on the anode side. The drying temperature has been varied between 22°C (ambient air temperature), 110°C, 150°C, 180°C, 200°C and 250°C within a continuous convection dryer. Further, different drying profiles have been applied by comparing to hot plate drying method. All other process parameters have been kept constant. The catalyst layers with different drying temperatures have been tested in-situ by electrochemical operation of the MEA. For Aquivion® as ionomer, the polarization curves are shown in Figure 2 and indicate that drying temperatures above 150°C (glass transition temperature) would lead to significant current density losses at wet and dry conditions. Furthermore, there doesn’t seem to be an optimum drying temperature below the glass transition temperature. Therefore, the best compromise of production throughput and electrochemical performance is reached at a temperature of 150°C, which is near the glass transition temperature of the ionomer. [1] Park H-S, Cho Y-H, Cho Y-H, Jung CR, Jang JH, Sung Y-E. Performance enhancement of PEMFC through temperature control in catalyst layer fabrication. Electrochimica Acta 2007;53(2):763–7. [2] Huang D-C, Yu P-J, Liu F-J, Huang S-L, Hsueh K-L, Chen Y-C et al. Effect of Dispersion Solvent in Catalyst Ink on Proton Exchange Membrane Fuel Cell Performance. Int. J. Electrochem. Sci. International Journal 2011;6:2551–65. [3] Hasegawa N, Kamiya A, Matsunaga T, Kitano N, Harada M. Analysis of crack formation during fuel cell catalyst ink drying process. Reduction of catalyst layer cracking by addition of high boiling point solvent. Colloids and Surfaces A: Physicochemical and Engineering Aspects 2021:127153. [4] Alink R, Singh R, Schneider P, Christmann K, Schall J, Keding R et al. Full Parametric Study of the Influence of Ionomer Content, Catalyst Loading and Catalyst Type on Oxygen and Ion Transport in PEM Fuel Cell Catalyst Layers. Molecules (Basel, Switzerland) 2020;25(7). Figure 1