Publication date: 10th April 2024
Hexagonal perovskite-related oxides have been of significant interest in recent years for their potential applications in electrochemical devices, particularly as solid electrolytes in fuel cells and electrolysis cells. The anisotropy of proton migration in these materials has been susceptive to shown a critical role in their performance, but the underlying mechanisms and factors governing this anisotropy remain poorly understood. In this study, using the {0001}-plane preferentially oriented Ba5Er2Al2ZrO13 (BEAZ) hexagonal perovskite electrolyte supported cell as a model system, we reveal the anisotropic characteristics of the proton conduction behavior. By controlling the orientation of the grains in the BEAZ thin film via surface energy driven secondary grain growth phenomenon, we demonstrate that proton migration in BEAZ is more favorable in the lateral direction than in the vertical direction. More importantly, density-functional-theory calculations and ab-initio molecular dynamics simulations suggest that anisotropic proton migration in the lateral direction is preferred through the perovskite-like layer rather than the intrinsically oxygen-deficient layer. Our study demonstrates that an electrostatic neutral perovskite-like layer in hexagonal perovskite related oxide should not be overlooked as a key parameter for achieving higher proton conduction kinetics.
This work was supported by the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT (NRF-2021M3I3A1084931), and the Research and Development Program of the Korea Institute of Energy Research (Grant number C3-2406). This work was also partially supported by New Energy Core Technology Development Project (No. 20223030040080 and No. 20213030030150) of the Korea Institute of Energy Technology Evaluation and Planning (KETEP) grant funded by the Korea government Ministry of Trade, Industry and Energy.
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