Investigation of gas transport resistance in fuel cell catalyst layers via hydrogen limiting current measurements of CO-covered catalyst surfaces

The efficiency of fuel cell operation at high power strongly affects the total cost of ownership of fuel cell vehicles. Gas transport resistance at the cathode strongly suppresses efficiency during high-power operation. The resistance comprises Knudsen diffusion resistance in pores formed among the primary carbon aggregates and local gas transport resistance. The former is independent of the electrochemically active Pt surface area per geometrical electrode area (roughness factor: RF). The latter is proportional to the inverse of RF. Separate identification of these resistances in actual catalyst layers remains challenging because of experimental limitations. Herein, we propose a method that can identify the RF-dependent and RF-independent resistances separately using a single sample. RF can be controlled by partially covering the Pt surface by CO. The gas transport resistance can be ascertained from the hydrogen limiting current. Measuring the hydrogen limiting current at controlled CO coverages allows separate identification of the resistances. The RF-dependent resistance is separable further into ionomer/Pt interfacial resistance and permeation resistance through the ionomer thin film by combining the obtained ionomer-to-carbon weight ratio dependence of each resistance component with structural and electrochemical analyses. The separate resistances show the ionomer/Pt interfacial resistance to be dominant in the catalyst layer.