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Assessing Substitution Effects on Surface Chemistry by in Situ Ambient Pressure X-ray Photoelectron Spectroscopy on Perovskite Thin Films, BaCe x Zr 0.9- x Y 0.1 O 2.95 ( x = 0; 0.2; 0.9).
ACS Applied Materials & Interfaces 2018 October 32
Performance of proton-solid oxide fuel cells (H+ -SOFC) is governed by ion transport through solid/gas interfaces. Major breakthroughs are then intrinsically linked to a detailed understanding of how parameters tailoring bulk proton conductivity affect surface chemistry in situ, at an early stage. In this work, we studied proton and oxygen transport at the interface between H+ -SOFC electrolyte BaCe x Zr0.9- x Y0.1 O2.95 ( x = 0; 0.2; 0.9) thin films and the gas (100 mTorr of H2 O and O2 ) by using synchrotron-based ambient pressure X-ray photoelectron spectroscopy at operating temperature (>400 °C). We developed highly textured BaCe x Zr0.9- x Y0.1 O2.95 epitaxial thin films, which exhibit high level of in-plane proton conductivity, that is, up to 0.08 S cm-1 at 500 °C for x = 0.9. Upon applying 100 mTorr water partial pressure above 300 °C, major changes are observed only in the O 1s and Y 3d core level spectra, with a clear Zr/Ce ratio dependency. OH- formation is favored by Ce content while initiated near Y. Hydration is also associated with surface secondary phase growth comprising oxygen-under-coordinated yttrium and/or yttrium hydroxide. With BaCe0.2 Zr0.7 Y0.1 O2.95 , high levels of ionic conductivities and chemical stability are obtained as a result of the optimized surface reaction kinetics, with low activation energy barrier for proton transport while restraining formation of OH- /SO4 2- adsorb species.
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