Abstract
Oxygen reduction in a solid oxide fuel cell cathode involves a nonequilibrium process of coupled mass and heat diffusion and electrochemical and chemical reactions. These phenomena occur at multiple temporal and spatial scales, making the modeling, especially in the transient regime, very difficult. Nonetheless, multiscale models are needed to improve the understanding of oxygen reduction and guide cathode design. Of particular importance for long-term operation are microstructure degradation and chromium oxide poisoning both of which degrade cathode performance. Existing methods are phenomenological or empirical in nature and their application limited to the continuum realm with quantum effects not captured. In contrast, steepest-entropy-ascent quantum thermodynamics can be used to model nonequilibrium processes (even those far-from equilibrium) at all scales. The nonequilibrium relaxation is characterized by entropy generation, which can unify coupled phenomena into one framework to model transient and steady behavior. The results reveal the effects on performance of the different timescales of the varied phenomena involved and their coupling. Results are included here for the effects of chromium oxide concentrations on cathode output as is a parametric study of the effects of interconnect-three-phase-boundary length, oxygen mean free path, and adsorption site effectiveness. A qualitative comparison with experimental results is made.
Funding statement: Funding for this research was provided by the US Office of Naval Research under Award No. N00014-11-1-0266.
Acknowledgements:
We acknowledge Advanced Research Computing at Virginia Tech for providing the necessary computational resources and technical support that have contributed to this work (http://www.arc.vt.edu). The authors would like to acknowledge the ASME as the original publisher of portions of the material in this paper in the proceedings of the 2015 ASME International Mechanical Engineering Congress and Exposition (IMECE2015) where this work was initially presented [35].
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