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Wide proliferation of low temperature hydrogen fuel cell systems, a key partof the hydrogen economy, is hindered by degradation of the platinum cathodecatalyst. Here, we provide a device level assessment of the molecular scalecatalyst degradation phenomena, using advanced operando X-ray scatteringtomography tailored for device-scale imaging. Each cell component, includingthe catalyst, carbon support, polymer electrolyte, and liquid water can besimultaneously mapped, allowing for deep correlative analysis. Chemical andthermal gradients formed inside the operating fuel cell produce highlyheterogeneous degradation of the catalyst nanostructure, which can be linked tothe macroscale design of the flow field and water distribution in the cellmaterials. Striking differences in catalyst degradation are observed betweenoperating fuel cell devices and the liquid cell routinely used for catalyststability studies, highlighting the rarely studied but crucial impact of thecomplex operating environment on the catalyst degradation phenomena. Thisdegradation knowledge gap highlights the necessity of multimodal in situcharacterization of real devices when assessing the performance and durabilityof electrocatalysts.

Holistic Multi-scale Imaging of Oxygen Reduction Reaction Catalyst Degradation in Operational Fuel Cells