Obtaining high power density at low operating temperatures has been an ongoing challenge in solid oxide fuel cells (SOFC), which are efficient engines to generate electrical energy from fuels. Here we report successful demonstration of a thin-film three-dimensional (3-D) SOFC architecture achieving a peak power density of 1.3 W/cm(2) obtained at 450 °C. This is made possible by nanostructuring of the ultrathin (60 nm) electrolyte interposed with a nanogranular catalytic interlayer at the cathode/electrolyte interface. We attribute the superior cell performance to significant reduction in both the ohmic and the polarization losses due to the combined effects of employing an ultrathin film electrolyte, enhancement of effective area by 3-D architecture, and superior catalytic activity by the ceria-based interlayer at the cathode. These insights will help design high-efficiency SOFCs that operate at low temperatures with power densities that are of practical significance.
The role of grain boundaries on oxygen surface exchange in an oxide ion conductor is reported. Atomic‐scale characterization of the microstructure and chemical composition near the grain boundaries of gadolinia‐doped ceria (GDC) thin films show the segregation of dopants and oxygen vacancies along the grain boundaries using the energy dispersive spectroscopy in scanning transmission electron microscopy (STEM‐EDS). Kelvin probe microscopy is employed to verify the charge distribution near grain boundaries and shows that the grain boundary is positively charged, indicating a high concentration of oxygen vacancies. AC impedance spectroscopy on polycrystalline GDC membranes with thin interfacial layers with different grain boundary densities at the cathodes demonstrated that the cells with higher grain boundary density result in lower electrode impedance and higher exchange current density. These experimental evidences clearly show that grain boundaries on the surface provide preferential reaction sites for facilitated oxygen incorporation into the GDC electrolyte.
Nanocrystalline YDC thin films with grain-sizes ranging from 38 to 93-nm were prepared using pulsed laser deposition followed by thermal annealing. Ionic conductivity decreased up to four orders of magnitude as the grain size increased. Using energy-dispersive X-ray spectroscopy, we showed that the counter-intuitive reduction in conductivity with grain-size is likely due to dopant and impurity segregation near grain-boundaries. Spectroscopic evidence suggests that the blocking effect due to defect segregation is more dominant on ionic conductivity than the grainsizes.
Local accumulation and dissipation of charges on the surface of oxide ion conductors resulting from electric potentials were observed with conductive atomic force microscopy (AFM). After a negative bias was applied at the tip, a sequence of surface potential maps appeared compatible with electron injection onto the electrolyte surface. Applying a positive bias, in contrast, generated a positive surface charge adjacent to the tip contact area. This observation is consistent with the formation of oxide ion vacancies on the oxide surface. In addition, oxide ion conductivity at a low temperature range (100-200 degrees C) was obtained, and the activation energy for diffusion in gadolinia-doped ceria (GDC) was calculated as approximately 0.56 eV, implying that the majority of oxide ion vacancies diffuse on the surface rather than inside the bulk of the electrolyte.
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