Proton exchange membrane unitized regenerative fuel cells (PEM-URFCs) combine the ability to both produce power (in fuel cell mode) and generate fuel and oxidant (in electrolysis mode) from the same cell. Compared with discrete fuel cell and electrolyzer systems, URFCs provide the potential for lower mass, volume, and cost. The composition and structure of the bifunctional oxygen catalyst layer (CL), which facilitates the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) at the same electrode, significantly affects performance and stability, particularly given the wide potential differences and different mass transport phenomena involved under operation in fuel cell or electrolysis mode. We previously showed bimetallic nanoframes provide bifunctional oxygen electrocatalysts with significantly higher activity compared with monometallic structures, evaluated using a rotating disk electrode configuration.¹ Here, we investigated the effects of the oxygen CL composition, loading, and spray parameters on the performance of URFC membrane electrode assemblies (MEAs). Pt black and IrO₂ catalysts were combined at different ratios and deposited at different mass loadings. Catalyst layers were sprayed directly onto membranes using an ultrasonic spray system. Within ultrasonically sprayed catalyst layers, higher spray rates resulted in improved fuel cell performance. Higher catalyst loadings improved both fuel cell and electrolyzer performance, but reached a region of diminishing returns at higher loadings. The ratio of the ORR catalyst (Pt) to the OER catalyst (IrO₂) modulated the performance in both fuel cell and electrolyzer modes. Different catalyst ratios influence the catalyst utilization at higher loadings. The comparison of URFC performance at same Pt or IrO₂ loadings indicates that in addition to the active catalyst itself, the non-catalytically active component influences MEA performance. This result is in line with our previous evaluation of synergistic effects of Pt and IrO₂ within rotating disk electrode measurements¹ and supports that in addition to the significant effects of catalyst material structure on performance, the electrode structure plays a critical role in fuel cell and electrolyzer performance in URFC MEAs. Repeated switching of URFC MEAs between fuel cell and electrolysis modes indicates that reasonable performance is maintained over the initial cycles within our single cell test configuration.

References

1. Godínez-Salomón, F.; Albiter, L.; Mendoza-Cruz, R.; Rhodes, C.P. Bimetallic Two-dimensional Nanoframes: High Activity Acidic Bifunctional Oxygen Reduction and Evolution Electrocatalysts. ACS Appl. Energy Mater. 2020, 3, 2404-2421. http://dx.doi.org/10.1021/acsaem.9b02051