Quantitative characterization and modeling of the microstructure of solid oxide fuel cell composite electrodes

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Zhang, Shenjia
Gokhale, Arun M.
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Three-phase porous composites containing electrolyte (ionic conductor), electronic conductor, and porosity phases are frequently used for solid oxide fuel cell (SOFC) electrodes. Performance of such electrodes is microstructure sensitive. Topological connectivity of the microstructural phases and total length of triple phase boundaries are the key microstructural parameters that affect the electrode performance. These microstructural attributes in turn depend on numerous process parameters including relative proportion, mean sizes, size distributions, and morphologies of the electrolyte and electronic conductor particles in the powder mix used for fabrication of the composites. Therefore, improvement of the performance of SOFC composite electrodes via microstructural engineering is a complex multivariate problem that requires considerable input from microstructure modeling and simulations. This dissertation presents a new approach for geometric modeling and simulation of three-dimensional (3D) microstructure of three-phase porous composites for SOFC electrodes and provides electrode performance optimization guidelines based on the parametric studies on the effects of processing parameters on the total length and topological connectivity of the triple phase boundaries. The model yields an equation for total triple phase boundary length per unit volume (LTPB) that explicitly captures the dependence of LTPB on relative proportion of electrolyte and electronic conductor phases; volume fraction of porosity; and mean size, coefficient of variation, and skewness of electrolyte and electronic conductor particle populations in the initial powder mix. The equation is applicable to electrolyte and electronic conductor particles of any convex shapes and size distributions. The model is validated using experimental measurements performed in this research as well as the measurements performed by other researchers. Computer simulations of 3D composite electrode microstructures have been performed to further validate the microstructure model and to study topological connectivity of the triple phase boundaries in 3D microstructural space. A detailed parametric analysis reveals that (1) non-equiaxed plate-like, flake-like, and needle-like electrolyte and electronic conductor particle shapes can yield substantially higher LTPB; (2) mono-sized electrolyte and electronic conductor powders lead to higher LTPB as compared to the powders having size distributions with large coefficients of variation; (3) LTPB is inversely proportional to the mean sizes of electrolyte and electronic conductor particles; (4) a high value of LTPB is obtained at the lowest porosity volume fraction that permits sufficient connectivity of the pores for gas permeability; and (5) LTPB is not sensitive to the relative proportion of electrolyte and electronic conductor phases in the composition regime of interest in composite electrode applications.
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