Impact of Electrode Thick Spot Irregularities on Polymer Electrolyte Membrane Fuel Cell Performance
Authors: Wang Min , Rome Grace , Medina Samantha , Pfeilsticker Jason , Kang Zhenye , Pylypenko Svitlana , Ulsh Michael , Bender Guido 
Published: December 2020

Polymer electrolyte membrane fuel cells (PEMFC) have great potential for power generation in many applications, but to implement them on a larger scale, understanding of quality requirements, tolerances, and controls during manufacturing must improve. As part of this broad challenge, irregularities resulting from the membrane electrode assembly (MEA) production process must be studied to determine if they impact the performance of the cell.1,2 One potential irregularity is a locally increased thickness of the coated or deposited electrode. In order to understand and provide insight into the impact of such irregularities, we intentionally created thick spots in the center of cathode electrodes, either by liquid casting or ultrasonic spraying of the additional catalyst ink. The thick spots fabricated by these two different approaches exhibited different sizes, morphologies, and Pt loading distributions, which were carefully characterized by optical microscopy, X-ray fluorescence spectroscopy (XRF), and scanning electron microscopy (SEM). Edge-protected MEAs were fabricated using both pristine electrodes and electrodes with thick spot irregularities. The effect of these irregularities on MEA structure were investigated by cross-sectional SEM. Electrochemical performance, including electrochemically active surface area (ECSA), H2/O2 polarization curves, mass activity and H2/air polarization curves, was measured to study the impact of the electrode irregularities on catalyst utilization and PEMFC initial performance. NREL’s segmented cell was utilized to investigate the resulting spatial performance of a representative thick spot MEA.

The results indicate that thick spot irregularities that are present in the center of the cathode electrode impact initial cell performance although the impact of the thick spots on ECSA and mass activity was minimal. The latter suggests that the number of active Pt sites and the kinetics were not significantly altered. However, the H2/air polarization curves indicated that liquid-cast thick spots and large sprayed thick spots decrease cell performance dramatically at current densities above 0.8 A/cm2. Based on cross-sectional SEM analysis, the likely causes of this performance drop may originate from (i) delamination between the GDL and CL, (ii) the presence of thin spots in the membrane due to deformation associated with the thick spot, (iii) additional compression of the GDL and/or (iv) thick catalyst layer sections inhibiting local mass transport. Spatial performance diagnostics confirmed that the performance loss of MEAs containing liquid-cast thick spots is more pronounced at high current density than at low current density. Moreover, the performance of the area surrounding the liquid-cast thick spot is impacted as well, likely due to the various morphological changes resulting from the irregularity. We expect that the morphological changes resulting from these irregularities could serve as seed points for premature cell failure in long-term PEMFC operation. Future work will focus on the impact of electrode thick spot irregularities on PEMFC performance-over-time and lifetime, for both reinforced and non-reinforced membranes.

References:

(1) Phillips, A.; Ulsh, M.; Porter, J.; Bender, G. Utilizing a Segmented Fuel Cell to Study the Effects of Electrode Coating Irregularities on PEM Fuel Cell Initial Performance. Fuel Cells
2017, 17 (3), 288–298. https://doi.org/10.1002/fuce.201600214.

(2) Phillips, A.; Ulsh, M.; Neyerlin, K. C.; Porter, J.; Bender, G. Impacts of Electrode Coating Irregularities on Polymer Electrolyte Membrane Fuel Cell Lifetime Using Quasi In-Situ Infrared Thermography and Accelerated Stress Testing. Int. J. Hydrogen Energy
2018, 43 (12), 6390–6399. https://doi.org/https://doi.org/10.1016/j.ijhydene.2018.02.050.

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