- Khedekar, Kaustubh;
- Zaffora, Andrea;
- Santamaria, Monica;
- Coats, Matthew;
- Pylypenko, Svitlana;
- Braaten, Jonathan;
- Atanassov, Plamen;
- Tamura, Nobumichi;
- Cheng, Lei;
- Johnston, Christina;
- Zenyuk, Iryna V
Fuel cell heavy-duty vehicles (HDVs) require increased durability of oxygen-reduction-reaction electrocatalysts, making knowledge of realistic degradation mechanisms critical. Here identical-location micro-X-ray fluorescence spectroscopy was performed on membrane electrode assemblies. The results exposed heavy in-plane movement of electrocatalyst after HDV lifetime, suggesting that electrochemical Ostwald ripening may not be a local effect. Development of local loading hotspots and preferential movement of electrocatalyst away from cathode catalyst layer cracks was observed. The heterogeneous degradation exhibited by a modified cathode gas diffusion layer membrane electrode assembly after HDV lifetime was successfully quantified by the identical-location approach. Further synchrotron micro-X-ray diffraction and micro-X-ray fluorescence experiments were performed to obtain the currently unknown correlation between electrocatalyst nanoparticle size increase and loading change. A direct correlation was discovered which developed only after HDV lifetime. The work provides a route to engineer immediate system-level mitigation strategies and to develop structured cathode catalyst layers with durable electrocatalysts. [Figure not available: see fulltext.]