Journal
INORGANIC CHEMISTRY
Volume 59, Issue 8, Pages 5339-5349Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.9b03417
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Funding
- Fond Franco-Canadien pour la Recherche (FFCR)
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The OP4-(Li/Na)(x)CoO2 phase is an unusual lamellar oxide with a 1:1 alternation between Li and Na interslab spaces. In order to probe the loca structure, electronic structure, and dynamics, Li-7 and Na-23 magic angle spinning nuclear magnetic resonance (MAS NMR) spectroscopy was performed in complementarity to X-ray diffraction and electronic and magnetic properties measurements. Li-7 MAS NMR showed that NMR shifts result from two contributions: the Fermi contact and the Knight shifts due to the presence of both localized and delocalized electrons, which is really unusual. Li-7 MAS NMR clearly shows several Li environments, indicating that, moreover, Co ions with different local electronic structures are formed, probably due to the arrangement of the Na+ ions in the next cationic layer. Na-23 MAS NMR showed that some Na+ ions are located in the Li layer, which was not previously considered in the structural model. The Rietveld refinement of the synchrotron XRD led to the OP4-[Li-0.42 Na-0.05]Na-0. 32 CoO2 formula for the material. In addition, Li-7 and Na-23 MAS NMR spectroscopies provide information about the cationic mobility in the material: Whereas no exchange is observed for Li-7 up to 450 K, the Na-23 spectrum already reveals a single average signal at room temperature due to a much larger ionic mobility.
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