Publication date: 10th April 2024
Space charge layers are common at heterogeneous interfaces [1]. Previous investigations [2-4] into the space charge layer (scl) effects at the interface between metal electrodes and proton-conducing electrolytes were predominantly done by the Distribution of Relaxation Times (DRT) method due to the challenge of distinguishing between various transfer processes through impedance spectroscopy. In the present study, the presence of a space charge layer at the interface between Ag electrodes and proton-conducting perovskite electrolytes of BaZr0.9Y0.1O3-δ (BZY10) is evidenced by a well separated semicircle from impedance spectra with characteristic capacitance of ~10-7 F.
The specific conductivities of grain boundaries and the Ag-BZY10 interface space charge layer were calculated on the basis of an ideal brick layer model and measured capacitances. Based on the Mott–Schottky approximation [5], the space charge layer potential, also known as the Schottky potential, was calculated for grain boundaries and the electrode interface vs temperature (300 – 550ºC), pO2 (10-5 – 0.98 atm) and pH2O (0.005 – 0.021 atm).
The Schottky potential at the electrode-electrolyte interface was found to be around 2 times higher than that of the grain boundaries, which for instance may arise from the segregation of protons at the interface in order to reduce the large lattice mismatch between the metal electrode and the perovskite oxide electrolyte. The potential increased with increasing pH2O for both grain boundaries and the Ag-BZY10 interface. The grain boundary potential decreased with increasing temperature, while pO2 had little effect. For the Ag-BZY10 interface potential, there was an apparent interplay between the effects of temperature and pO2. Interpretations of the above phenomena will be proposed and discussed.
The China Scholarship Council is acknowledged for the doctoral scholarship of Yabing Wen (202008320294).
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