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首页> 外文期刊>RSC Advances >Utilizing non-stoichiometry in Nd2Zr2O7 pyrochlore: exploring superior ionic conductors
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Utilizing non-stoichiometry in Nd2Zr2O7 pyrochlore: exploring superior ionic conductors

机译：利用ND2ZR2O7烧画中的非化学计量：探索优质离子导线

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摘要

To explore materials with high ionic conductivity without any heterovalent substitution, a non-stoichiometric Nd _(2?x) Zr _(2+x) O _(7+x/2) (?0.2 ≤ x ≤ 0.4) pyrochlore system was synthesized via a combustion process. All the compositions were characterized by X-ray diffraction and revealed perfect pyrochlore-type compounds. Interestingly, Raman spectroscopy exhibited an enhanced oxygen disorder in Nd _(1.6) Zr _(2.4) O _(7.2) ( x = 0.4) relative to the rest of the compositions, which was manifested in a substantially high pre-exponential factor for this composition. Detailed AC impedance analysis revealed that the ionic conductivity for Nd _(1.6) Zr _(2.4) O _(7.2) was higher by two orders of magnitude despite the similar structures adopted by all the other compositions. X-ray photoelectron spectroscopy provided support for the high ionic conductivity observed. Modulus spectroscopic analysis related the microscopic energy barrier to the macroscopic activation energy. The highlight of the study was the high ionic conductivity (1.78 × 10 ~(?2) S cm ~(?1) at 973 K) for Nd _(1.6) Zr _(2.4) O _(7.2) , which is comparable to the highest values reported for a zirconia-based system at this temperature. This was attributed to the optimized hybrid structure consisting of fluorite-type disordered zones interspersed in the ordered pyrochlore structure obtained under suitable annealing conditions. The present study highlights the utilization of non-stoichiometry in the pyrochlore structure to tailor its ionic conductivity. Such high ionic conductivity observed in Nd _(1.6) Zr _(2.4) O _(7.2) makes it a superior candidate for electrolyte materials as it is endowed with the stability of zirconia-based systems and has ionic conductivity comparable to ceria-based systems.
机译：为了探索具有高离子电导率的材料而没有任何异常取代，非化学计量Nd _（2×x）zr _（2 + x）o _（7 + x / 2）（Δ0.2≤x≤0.4）pyrochlore系统是通过燃烧过程合成。所有组合物的特征在于X射线衍射，并揭示了完美的纤维型化合物。有趣的是，拉曼光谱相对于其余组合物的Nd _（1.6）Zr _（2.4）O _（2.4）（x = 0.4）表现出增强的氧气病症，其表现为基本上高的预指数因子这个组成。详细的AC阻抗分析表明，尽管所有其他组合物采用的类似结构，但Nd _（1.6）Zr _（2.4）Zr _（2.4）O _（7.2）的离子电导率较高了两个数量级。 X射线光电子能谱提供了对观察到的高离子电导率的支持。模量光谱分析与宏观激活能量的微观能量屏障。该研究的亮点是Nd _（1.6）Zr _（2.4）O _（7.2）的高离子电导率（1.78×10〜（Δ2）Cm〜（α1）），其可比较在此温度下为基于氧化锆的系统报告的最高值。这归因于优化的混合结构，其由散射在合适的退火条件下获得的有序的纤维结构结构中的萤石型无序区域组成。本研究强调了在柏树林结构中利用非化学计量来定制其离子电导率。在Nd _（1.6）Zr _（2.4）O _（7.2）中观察到的这种高离子电导率使其成为电解质材料的优异候选者，因为它具有基于氧化锆的系统的稳定性并且具有与基于Ceria的离子电导率相当系统。

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