Model Based Comparative Analysis of GDC and YSZ Based Solid Oxide Fuel Cells

Designing solid oxide fuel cell (SOFCs) stacks for transportation applications places new challenges on SOFC architecture and operation with respect to power density, dynamic response, and thermal management. Recent developments in SOFCs with either thin-film yttria stabilized zirconia (YSZ) electrolytes (thickness ≤ 5 μm) or highly conductive, gadolinia-doped ceria (GDC) electrolytes (thicknesses ≥10 μm) enable thigh-power-density stack operation at inlet temperatures well below 700ºC with the potential for using compliant seals and lower cost ferrous interconnect materials. Applications, such as hybridized aircraft engines, can use such SOFC stacks if they meet strict requirements with respect to specific power and thermal management. Highly conductive GDC-based electrolytes offer pathways to high power-density SOFCs at operating temperatures below 650ºC, but the rise in mixed ionic electronic conductivity (MIEC) above 650ºC reduces open circuit voltages and thus fuel cell efficiency [1,2]. This necessitates thermal management to maintain operating temperatures and mitigate thermo-mechanical stresses within an SOFC. Thin-film YSZ electrolytes offer lower power densities below 650ºC, but avoid the penalties associated with MIEC behavior at higher temperatures and therefore reduce the challenges associated with thermal management at high power densities. In this work, a model-based approach is used to compare SOFC stack operation with thin-film YSZ electrolytes and with GDC-based electrolytes for operation on hydrogen and reformate fuels at high-power densities relevant for transportation applications. To calibrate models to experimental cell performance, polarization curves of a commercially available YSZ-based cell operating between 600-750ºC and of a high-power-density GDC cell operating between 500-650ºC are used to fit electrochemical model parameters for both electrolytes. Modeling of the YSZ based cell can neglect electronic charge transfer through the membrane electrolyte, but GDC-cell modeling must account for the multiple charge carriers (ceria polarons and oxygen vacancies) in the electrolyte [3]. Electrochemical parameters for ionic conductivities and electrochemical reaction rate parameters for oxide cathodes and nickel-electrolyte-composite anodes are fit to the experimental polarization data over the broad range of operating temperatures. Global rate expressions to account for internal reforming on the active nickel surfaces of anode are adopted from literature [4,5]. The calibrated cell model for each cell type is adopted to a down-the-channel discretized cell simulation to predict heat loss and temperature gradients at high current densities. This presentation compares GDC- and YSZ-based SOFCs in high power-density applications from fundamental and practical perspectives. The open-circuit voltages for GDC-based cells drops with increasing temperature to about 0.85 V/cell at 650°C which is lower than the Nernst open-circuit voltage of YSZ-based cells (≥ 1.05 V/cell) at similar conditions. Both types of cells can sustain power densities around 1.0 W/cm 2 with high excess cathode air ratios ≥ 5 to keep temperature gradients near 10°C/cm. These results show that GDC-based cells support higher power densities at lower cell flow inlet temperatures < 600°C, whereas thin-film YSZ cells provide superior performance at flow inlets that drive cell temperatures > 600°C. Higher stack power densities > 1.0 W/cm 2 must be supported by stack designs that alleviate high thermal stresses and allow steeper gradients of temperature. A summary of stack design and operational strategies that meet the stringent requirements of high power-density operation will be presented in the light of the modeling resuls.. References: [1] Wachsman, E. D., & Lee, K. T. (2011). Lowering the temperature of solid oxide fuel cells. Science , 334 (6058), 935–939. [2] Inaba, H., & Tagawa, H. (1996). Ceria-based solid electrolytes. Solid State Ionics, 83, 1-16. [3] Zhu, H., Ricote, S., Coors, W. G., Chatzichristodoulou, C., & Kee, R. J. (2014). Equilibrium and transient conductivity for gadolium-doped Ceria under large perturbations: II. modeling. Solid State Ionics , 268 , 198–207. [4] Timmermann, H., Sawady, W., Reimert, R., & Ivers-Tiffée, E. (2010). Kinetics of (reversible) internal reforming of methane in solid oxide fuel cells under stationary and Apu Conditions. Journal of Power Sources , 195 (1), 214–222. [5] Van Biert, L., Visser, K., & Aravind, P. V. (2019). Intrinsic methane steam reforming kinetics on nickel-ceria solid oxide fuel cell anodes. Journal of Power Sources , 443 , 227261. https://doi.org/10.1016/j.jpowsour.2019.227261