Challenges in low-temperature fuel cells
Gallagher, Kevin Gregory
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Low-temperature fuel cells (LTFC) such as phosphoric acid fuel cells (PAFC) and proton exchange membrane fuel cells (PEMFC) are a promising electrochemical energy system for the conversion of hydrogen to electricity. Many challenges must be overcome before commercialization is possible. This dissertation focuses on the degradation of carbon catalyst supports and PEMFC water management. Kinetic studies are presented on the structure-reactivity relationship including an in-depth study of commercially available and model carbons. A mechanism and numerical model of the electrochemical oxidation of graphene-based carbon is proposed to explain longstanding questions. Three mechanisms are concluded to contribute to the current decay commonly observed during electrochemical oxidation: mass loss, reversible passive oxide formation, and irreversible oxide formation. Water uptake and electro-osmosis are investigated to improve the understanding and aid modeling of water transport in PEMFCs below 0 °C. The implication of an electro-osmotic drag coefficient less than unity is discussed in terms of proton transport mechanisms. Capillary pressure saturation relations are presented for carbon fiber paper which can both be used as gas-diffusion layers in PEMFCs. Boundary and scanning curves for imbibition and drainage are measured to further understanding of the hysteresis observed during PEMFC operation.