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A review of defect structure and chemistry in ceria and its solid solutions.
Chemical Society Reviews ( IF 46.2 ) Pub Date : 2019-12-24 , DOI: 10.1039/c9cs00588a
Rafael Schmitt 1 , Andreas Nenning 2 , Olga Kraynis 3 , Roman Korobko 4 , Anatoly I Frenkel 5 , Igor Lubomirsky 3 , Sossina M Haile 6 , Jennifer L M Rupp 7
Affiliation  

Ceria and its solid solutions play a vital role in several industrial processes and devices. These include solar energy-to-fuel conversion, solid oxide fuel and electrolyzer cells, memristors, chemical looping combustion, automotive 3-way catalysts, catalytic surface coatings, supercapacitors and recently, electrostrictive devices. An attractive feature of ceria is the possibility of tuning defect-chemistry to increase the effectiveness of the materials in application areas. Years of study have revealed many features of the long-range, macroscopic characteristics of ceria and its derivatives. In this review we focus on an area of ceria defect chemistry which has received comparatively little attention - defect-induced local distortions and short-range associates. These features are non-periodic in nature and hence not readily detected by conventional X-ray powder diffraction. We compile the relevant literature data obtained by thermodynamic analysis, Raman spectroscopy, and X-ray absorption fine structure (XAFS) spectroscopy. Each of these techniques provides insight into material behavior without reliance on long-range periodic symmetry. From thermodynamic analyses, association of defects is inferred. From XAFS, an element-specific probe, local structure around selected atomic species is obtained, whereas from Raman spectroscopy, local symmetry breaking and vibrational changes in bonding patterns is detected. We note that, for undoped ceria and its solid solutions, the relationship between short range order and cation-oxygen-vacancy coordination remains a subject of active debate. Beyond collating the sometimes contradictory data in the literature, we strengthen this review by reporting new spectroscopy results and analysis. We contribute to this debate by introducing additional data and analysis, with the expectation that increasing our fundamental understanding of this relationship will lead to an ability to predict and tailor the defect-chemistry of ceria-based materials for practical applications.

中文翻译:

二氧化铈及其固溶体的缺陷结构和化学综述。

Ceria及其固体解决方案在多种工业过程和设备中起着至关重要的作用。这些包括太阳能到燃料的转换,固体氧化物燃料和电解池,忆阻器,化学循环燃烧,汽车三元催化剂,催化表面涂层,超级电容器以及最近的电致伸缩设备。氧化铈的一个吸引人的特征是可以调整缺陷化学成分,以提高材料在应用领域的有效性。多年的研究揭示了二氧化铈及其衍生物的远距离,宏观特性的许多特征。在这篇综述中,我们关注的是氧化铈缺陷化学领域,该领域受到的关注相对较少-缺陷引起的局部畸变和短距离关联。这些特征本质上是非周期性的,因此不易通过常规的X射线粉末衍射检测到。我们汇编通过热力学分析,拉曼光谱和X射线吸收精细结构(XAFS)光谱获得的相关文献数据。这些技术中的每一种都可以提供对物质行为的洞察力,而无需依赖长期的周期性对称性。从热力学分析,可以推断出缺陷的关联。通过XAFS(一种元素特定的探针),可以获得选定原子物种周围的局部结构,而通过拉曼光谱法,则可以检测到局部对称性断裂和键合模式的振动变化。我们注意到,对于未掺杂的二氧化铈及其固溶体,短程有序与阳离子-氧-空位配位之间的关系仍然是活跃的辩论主题。除了整理文献中有时相互矛盾的数据外,我们还通过报告新的光谱学结果和分析来加强本综述。我们通过引入其他数据和分析来为这场辩论做出贡献,并期望增进对这种关系的基本理解将能够预测和定制用于实际应用的二氧化铈基材料的缺陷化学。
更新日期:2020-02-13
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