Publication date: 10th April 2024
Structural features of materials, such as lattice distortions, water uptake, and oxide vacancies, are key factors that define protonic conduction. It is also worth noting that fast oxygen diffusion is advantageous for hydration kinetics since proton incorporation requires the migration of oxygen vacancies.
Here, a combination of 18O tracer isotopic exchange and Secondary Ion Mass Spectrometry (SIMS) measurements was applied to obtain oxygen surface exchange and diffusion coefficients of BaCe0.8Y0.1Yb0.1O3-δ (BCYYb), BaSn0.8Y0.1Yb0.1O3-δ (BSYYb), and BaZr0.8Y0.1Yb0.1O3-δ (BZYYb). The isotopic exchange was conducted in dry (18O2) and wet (H218O) atmospheres at various temperatures. Lower oxygen diffusion coefficients were observed for the wet exchange, indicating that the humidified and dry atmospheres affect oxygen transport differently. In some cases, variations in the surface exchange and diffusion coefficients were observed at the phase transition temperature, suggesting a different rate-limiting step in the oxygen exchange and diffusion processes. Oxygen diffusivity was correlated to the conductivity measured by impedance spectroscopy (EIS), and the equilibrium constants associated with water incorporation were derived from thermogravimetric analysis (TGA) in the temperature range 100-900 °C under a water partial pressure of 0.023 atm. The constants, calculated under the assumption of a negligible hole concentration, were linear in the Arrhenius plot. In contrast, high-temperature X-ray diffraction (XRD) revealed complex structural transitions. The structural changes linked to the water uptake were confirmed by Raman spectroscopy carried out at variable temperatures under dry and wet atmospheres. Results were in good agreement with data reported by Grimaud et al [1]. for BaCe0.9Y0.1O3-d, although the detection of OH bands using Raman spectroscopy remains an open discussion.
This work was supported by the French National Research Agency (ANR) as part of the AAPG2021 - CES50 call (ANR-20-CE05-0001).
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