Significant Reduction in Hydration Energy for Yttria Stabilized Zirconia Grain Boundaries and the Consequences for Proton Conduction
Significant Reduction in Hydration Energy for Yttria Stabilized Zirconia Grain Boundaries and the Consequences for Proton Conduction
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DOI：
10.1021/la501860k
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发表时间：
2014-09-02
期刊：
影响因子：
3.9
通讯作者：
Tanaka, Isao
中科院分区：
文献类型：
--
作者：
Dawson, James A.;Tanaka, Isao
使用完善的原子技术，我们调查的缺陷化学，结构效应，和能量的质子掺入在西格玛5（310）/[001]和西格玛5（210）/[001]对称倾斜晶界的氧化钇稳定的氧化锆。在过去的工作的基础上，我们始终显示出显着的减少（类似于4-5 eV）的质子掺入和水化能在晶界结构和周围的散装材料和未掺杂的ZrO 2晶界获得的值相比。这种降低在Y偏析的晶界和Y的分布完全随机的晶界中都是普遍的。正如许多实验研究所报告的那样，这里呈现的结果强烈支持了该系统中的质子传导主要是界面驱动的论点。氧化还原性能也提出了晶界结构和缺陷偏析。这里提出的方法和结果也可以应用到广泛的质子导体，并将证明在任何未来的评估晶界上的缺陷化学质子在这些系统中的影响是必不可少的。
Using well-established atomistic techniques, we investigate the defect chemistry, structural effects, and energetics of proton incorporation at the Sigma 5(310)/[001] and Sigma 5(210)/[001] symmetrical tilt grain boundaries of yttria-stabilized zirconia. Building upon past work, we consistently show a dramatic decrease (similar to 4-5 eV) in the proton incorporation and hydration energies in and around the grain boundary structures compared to values obtained for the bulk material and undoped ZrO2 grain boundaries. This decrease is prevalent in both Y segregated grain boundaries and grain boundaries where the distribution of Y is completely random. The results presented here strongly support the argument that proton conduction in this system is primarily interfacially driven, as reported by numerous experimental studies. Redox properties are also presented for grain boundaries structures both with and without defect segregation. The methodology and results presented here can also be applied to a wide range of proton conductors and will prove essential in any future assessment of the effects of grain boundaries on the defect chemistry of protons in these systems.