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Factors that Influence Cation Segregation at the Surfaces of Perovskite Oxides

机译:影响钙钛矿表面阳离子偏析的因素

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As the oxygen reduction reaction (ORR) becomes more critical for development of solid oxide fuel cells (SOFCs) that operate at 500- 700°C, the correlation between the surface chemistry and electrochemical performance is important to understand and enable design of cathode materials with optimal surface chemistry. Recently we demonstrated that elastic and electrostatic interactions of the dopant with the host lattice drive dopant segregation, a detrimental process on the surface of perovskite cathodes (1). Motivated by those results, here we investigated the effects of Asite stoichiometry in La_(0.8)Sr_(0.2)MnO_3 (LSM) thin films on the surface chemistry and electrochemical activity. Angle-resolved Xray photoelectron spectroscopy was employed to identify the surface cation content and chemical bonding states. A-site deficient LSM films showed higher chemical stability against Sr segregation and secondary phase formation upon annealing. This was correlated with a higher electrochemical activity measured by AC impedance spectroscopy. Given the insulating nature of secondary phases created on the surface upon annealing, observed higher electrochemical stability in A-site deficient LSM films can be ascribed to the suppressed surface segregation and phase separation.
机译:随着氧还原反应(ORR)对于在500-700℃下操作的固体氧化物燃料电池(SOFC)变得更为关键,表面化学和电化学性能之间的相关性对于理解和实现阴极材料的设计是重要的最佳表面化学。最近,我们证明掺杂剂的弹性和静电相互作用与主晶格驱动掺杂剂偏析,在钙钛矿阴极(1)表面上的损害过程(1)。通过这些结果的激励,在这里,我们研究了在表面化学和电化学活性上的La_(0.8)Sr_(0.2)MnO_3(LSM)薄膜中的LA_(0.8)SR_(0.2)MNO_3(LSM)薄膜的影响。角度分辨的X射线光电子能谱被用来鉴定表面阳离子含量和化学粘合状态。 A现场缺陷的LSM薄膜在退火时显示出对SR偏析和二次相形成的较高的化学稳定性。这与通过AC阻抗光谱法测量的更高电化学活性相关。考虑到在退火时在表面上产生的二次相的绝缘性质,观察到的A现场缺陷的LSM膜中的更高的电化学稳定性可以归因于抑制的表面偏析和相分离。

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