Protonic defects in yttria stabilized zirconia : incorporation, trapping and migration
Protonic defects in yttria stabilized zirconia : incorporation, trapping and migration
复制标题
氧化钇稳定氧化锆中的质子缺陷：掺入、捕获和迁移
DOI：
10.1039/c4cp00021h
复制
发表时间：
2014
期刊：
影响因子：
--
通讯作者：
Hungru Chen and Isao Tanaka
中科院分区：
文献类型：
--
作者：
James A. Dawson;Hungru Chen and Isao Tanaka
经典和量子力学模拟技术已被应用于调查的掺入，迁移和潜在的结合体氧化钇稳定的氧化锆（YSZ）的质子缺陷。计算的氧化还原反应能量被认为是高的，虽然还原能低于散装立方氧化锆，并示出进一步降低，随着Y含量的增加。YSZ的水化能也低于大块ZrO 2的计算值，并且当氧离子与至少一个Y离子非常接近时，发现水化能最低。强结合（质子捕获）的能量之间的质子和额外的受体掺杂剂，包括Sc，Yb和Gd观察。这些能量被发现显着不同，这取决于当地的配置，并再次普遍低于ZrO 2的值。密度泛函理论（DFT）计算用于确定质子通过相邻氧离子转移的能垒（Grötthuss型机制）。能量势垒为0.32-0.42 eV的最接近的O-O原子间距离的路径，并被发现是非常具有可比性的完善的质子传导材料。
Both classical and quantum mechanical simulation techniques have been applied to investigate the incorporation, migration and potential binding of protonic defects in bulk yttria-stabilised zirconia (YSZ). The calculated redox reaction energies are found to be high, although the reduction energies are lower than those of bulk cubic ZrO2 and are shown to decrease further with increasing Y content. The hydration energies for YSZ are also lower than the values calculated for bulk ZrO2 and are found to be lowest when the oxygen ion is in close proximity to at least one Y ion. Strong binding (proton trapping) energies are observed between the protons and additional acceptor dopants including Sc, Yb and Gd. These energies are found to vary significantly depending on local configuration and again are generally lower than the values for ZrO2. Density functional theory (DFT) calculations are used to determine energy barriers for proton transfers via neighbouring oxygen ions (Grötthuss-type mechanism). Energy barriers of 0.32–0.42 eV are obtained for the pathways with the closest O–O interatomic distances and are found to be very comparable to well-established proton conducting materials.