Journal
JOURNAL OF MATERIALS CHEMISTRY A
Volume 5, Issue 47, Pages 25044-25055Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c7ta08733k
Keywords
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Funding
- French National Research Agency (ANR) as a part of the Investissements d'Avenir program [ANR-10-EQPX-45, 20160282]
- FEDER
- Region Hauts-de-France
- RS2E Network
- Region Nouvelle Aquitaine
- French National Research Agency (STORE-EX Labex Project) [ANR-10-LABX-76-01]
- French National Research Agency (HIPOLITE Progelec project) [ANR-12-PRGE-0005-02]
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Tavorite-type compositions offer rich crystal chemistry for positive electrodes in rechargeable batteries, among which (LiVPO4F)-P-III has the highest theoretical energy density (i.e. 655 Wh kg(-1)). In this article, we report for the first time the synthesis of the related Na-based phase crystallizing in the Tavorite-like structure. Its in-depth structural and electronic characterization was conducted by a combination of several techniques, spanning electron and X-ray powder diffraction as well as infrared and X-ray absorption spectroscopy. The magnetic susceptibility measurement reveals an average oxidation state for vanadium slightly higher than V3+. This slight oxidation is supported by infrared and X-ray absorption spectroscopies which highlight the presence of V4+ = O vanadyl-type defects leading to an approximated NaVIII (0.85)((VO)-O-IV)(0.15)(PO4)F-0.85 composition. In this material, the profile of the diffraction lines is governed by a strong strain anisotropic broadening arising from the competitive formation between the ionic V3+-F and the covalent V4+ = O bonds. This material shows a limited extraction of sodium, close to 15% of the theoretical capacity. Indeed, its electrochemical properties are strongly inhibited by the intrinsic low sodium mobility in the Tavorite framework.
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