Electrodes or catalyst layers (CLs) are the heart of fuel cell and electrolyzer cell devices. They are mainly heterogeneous porous electrodes composed of catalyst particles, ion-conducting polymer material, and void spaces that make up the triple-phase boundary (TPB). It is important to tailor the CL’s microstructure such that there are abundant TPBs where reactions take place to maximize catalyst utilization and improve cell performance. However, this is a critical challenge due to lack of fundamental understanding of the interfacial transport within the CL. Understanding how catalyst ink parameters affect ink properties and how ink components interact, and ultimately, their relationship with CL microstructure formation and cell performance, are essential to designing electrodes. Electrode morphology is important and is controlled by the ionomer/catalyst interactions formed in precursor inks that evolve during mixing and electrode fabrication.In this study, we probe interactions in catalyst inks with different formulations (ionomer-to-carbon ratio and IPA/water) using a new experimental method to unravel the complexities of ionomer/catalyst particle interactions. The new experimental method is a combination of rheological and electrical impedance spectroscopy measurements (rheo-EIS) that takes advantage of the dynamic nature of catalyst ink and the fact that the rheological and electrical behaviors of the ink are coupled to the microstructure of the material. Using rheo-EIS tool, in combination with zeta (ζ) potential and dynamic light scattering (DLS) measurements, we were able to systematically study how the level of agglomeration of the inks and microstructures evolve with respect to different I/C ratios, solvent formulation, and external shear forces. Results from the three-phase rebuilt test designed to simulate the ink coating condition with single-frequency EIS measurement give information on how the ionomer/catalyst particle interactions form and recover during the coating process. In addition, the full frequency range EIS measurements provide complementary data of the ionic and electrical resistance of the ink before and after high shear applications. Furthermore, the observations of the effect of I/C and IPA/water ratios from this study provide insights on how to better engineer suitable catalyst inks and how to control specific CL microstructure without the need for time-consuming optimization and empirical studies.
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