Abstract
Three types of CeO2–ZrO2 (Ce:Zr = 1:1 molar ratio) compounds with different oxygen storage/release capacity (OSC) were characterized by means of the Ce K-edge and Zr K-edge XAFS. In order to investigate the relationship between the OSC and local structure, the quantitative EXAFS curve-fitting analysis was applied. By enhancing the homogeneity of the Ce and Zr atoms in the CeO2–ZrO2 solid solution, the OSC performance increased. Additionally, from the XRD analysis, the homogeneous CeO2–ZrO2 solid solution has an ordered cation arrangement, and exhibits the highest OSC. The crystal structure of this CeO2–ZrO2 solid solution is usually termed as “κ-CeZrO4 phase”. However, the OSC performance of κ-CeZrO4 degrades upon a high-temperature treatment under an oxidative atmosphere. The fresh κ-CeZrO4 was aged at 973, 1,273 and 1,473 K under an oxidative atmosphere, respectively. The OSC performance deteriorated as: the fresh sample ≈973 > 1,273 > 1,473 K-aged samples. We also found that, if the temperature was beyond 1,273 K, the Ce/Zr ordered arrangement would collapse and the local structure around Ce and Zr ions would also changed remarkably. These results indicated that OSC was strongly dependent on its atomic structure.
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