Abstract

We investigated the atomic and local electronic structures of Ca2AlMnO5+δ to assess its potential as an oxygen storage material. High-angle annular dark-field scanning transmission electron microscopy was used to investigate structural changes in the material during oxygen storage. We found that the AlO4 tetrahedra convert to AlO6 octahedra during such a process. According to the Mn L-edge electron energy-loss near-edge structure (ELNES) measurements, the Mn oxidation state increased from +3 to +4 on oxygen storage. The observed site-resolved oxygen K-ELNES and first-principles electronic structure calculations showed that each nonequivalent oxygen site has different characteristics, corresponding to local chemical bonding and oxygen intake and release. For Ca2AlMnO5, the prepeak intensity was higher at MnO6 octahedral sites, indicating covalent bonding between the oxygen and Mn atoms. After oxygen storage, the ELNES spectra revealed that the Jahn–Teller distortion of the Mn sites was suppressed by the in...

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