Lifetime-limiting failure of fuel cell membranes is generally attributed to their chemical and/or mechanical degradation. Although both of these degradation modes occur concurrently during operational duty cycles, their uncoupled investigations can provide useful insights into their individual characteristics and consequential impacts on the overall membrane failure. X-ray computed tomography is emerging as an advantageous tool for fuel cell failure analysis due to its non-destructive and non-invasive 3D imaging capabilities at ambient conditions. In the present work, post-mortem failure analysis of pure mechanical and pure chemical membrane degradation modes is performed three-dimensionally using this technique. A uniquely comprehensive analysis afforded by this technique reveals that membrane failure is almost exclusively characterized by crack formations during mechanical degradation and by severe thinning accompanied by electrode shorting and pinhole formation during chemical degradation, respectively. Catalyst layer cracks, particularly on the cathode side, are found to interact strongly with mechanically induced membrane cracks. The conjoint effect of chemical and mechanical stressors is established as a necessary requirement for: (i) exclusive membrane crack development independent of catalyst layer cracks; and (ii) crack branching during membrane crack propagation. Overall, the membrane failure analysis improves its reliability and quantitative character with the adoption of 3D imaging. The transportation sector is a significant contributor to global greenhouse gas emissions and with ever-growing concerns around the global warming effect, research and development of novel clean energy based automotive solutions is being pursued worldwide. Hydrogen fuel cells have thus far emerged as a promising alternative to fossil fuel based internal combustion engines due to their clean, noisefree, and efficient operation.1 Polymer electrolyte membrane (PEM) fuel cells 2 are widely used in fuel cell electric vehicles (FCEVs) and supply electrical energy from the electrochemical conversion of hydrogen and oxygen (usually supplied as air) into water. In automotive applications, the fluctuating operating conditions due to vehicle dynamics, variations in loads and environmental conditions, startups and shutdowns, fuel starvation, contamination, and freeze-thaw cycles pose significant durability challenges for the PEM fuel cells.
3Understanding the specific durability problems and developing suitable solutions remains a key research focus in automotive PEM fuel cell technology research and is critical to the long-term and large-scale commercial adoption of this technology. Given the complex interplay of multiple physical phenomena that are simultaneously active in an operating PEM fuel cell, various deleterious factors affecting PEM fuel cell components can collectively lead to a gradual performance loss and eventual failure.In PEM fuel cells, the electrodes are separated by a polymeric membrane which allows selective tran...