In this work, as-received pristine GDLs were degraded (aged) through an accelerated ageing process by immersion into a 35% wt. solution of H 2 O 2 at 90 • C for 12 hours. Pristine and degraded GDLs were assembled in custom-built fuel cells for in operando synchrotron X-ray visualization. Electrochemical impedance spectroscopy (EIS) measurements were obtained, while synchrotron X-ray radiography was performed to investigate the effect of ageing on liquid water transport behavior. In both pristine and aged GDLs, the liquid water profile converged to an upper (terminal) threshold in the saturation pattern as the current density increased. The terminal steady state liquid water profile was established at a lower current density for the aged GDLs compared to that of the pristine GDLs. Higher water quantities of liquid water accumulated at the GDL/flow field channel and MPL/carbon fiber substrate interfaces of the fuel cell with an aged GDL compared to the fuel cell with a pristine GDL. The aged GDLs exhibited more liquid water accumulation at lower current densities. Increases in liquid water accumulation and reduced performance were attributed to the reduction in hydrophobicity of the GDL.

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In this thesis, the relative humidity (RH) of the cathode reactant gas was investigated as a factor which influences gas diffusion layer (GDL) liquid water accumulation and mass transport-related efficiency losses over a range of operating current densities in a polymer electrolyte membrane (PEM) fuel cell. Limiting current measurements were used to characterize fuel cell oxygen transport resistance while simultaneous measurements of liquid water accumulation were conducted using synchrotron X-ray radiography. GDL porosity distributions were characterized with micro-computed tomography (μCT). The work presented here can be used by researchers to develop improved numerical models to predict GDL liquid water accumulation and to inform the design of next-generation GDL materials to mitigate mass transport-related efficiency losses. This work also contributes an extensive set of concurrent performance and liquid water visualization data to the PEM fuel cell field that can be used for validating multiphase transport models.iii

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