On the hydration of grain boundaries and bulk of proton conducting BaZr_0.7Pr_0.2Y_0.1O_3-未

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• 作者：Kristine Bakkemo Kostø ; l ; Anna Magrasó ; Truls Norby ; ^{truls.norby@kjemi.uio.no}
• 关键词：BaZrO3 ; Pr-substituted ; acceptor-doped ; BaZr0.7Pr0.2Y0.1O3-未 ; Proton conductivity ; Grain boundaries ; space charge layer ; Hydration ; Impedance spectroscopy
• 刊名：International Journal of Hydrogen Energy
• 出版年：2012
• 期刊代码：42_03603199
• 类别：ch
• 出版时间：May, 2012
• 卷：37
• 期：9
• 页码：7970-7974
• 文件大小：423 K

摘要

We report here for the first time bulk and grain boundary conductivities from impedance spectra of a ceramic proton conductor (BaZr_0.7Pr_0.2Y_0.1O_3-未) taken during hydration and H/D isotope exchange transients (at 400聽掳C). The results suggest that water moves quickly along grain boundary cores, and then interact from there with the space charge layers and, in turn, grain interiors. Hydration and H/D isotope exchange have simple monotonic effects on the bulk conductivity in line with what is expected from it being dominated by protons. The transients for grain boundary conductivity exhibit however hysteresis: During hydration, the core charge and grain boundary resistance appear to go through transient minima related to non-equilibrium distributions of defects between the core and grain interior - notably because protons diffuse faster than oxygen vacancies between the grain boundary and grain interior. At equilibrium, hydration increases the core charge and the depletion of positive charge carriers in the space charge layers. During H/D isotope exchange relatively fast hysteretic transients indicate that the space charge layers experience changes in charge carrier (D⁺ vs. H⁺) mobility as well as in D₂O vs. H₂O hydration thermodynamics.