Complete three-electron vanadium redox in NASICON-type Na3VSc(PO4)3 electrode material for Na-ion batteries

T. I. Perfilyeva, O. A. Drozhzhin, A. M. Alekseeva, M. V. Zakharkin, A. V. Mironov, I. V. Mikheev, Z. V. Bobyleva, A. P. Marenko, A. V. Marikutsa, A. M. Abakumov, E. V. Antipov

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Abstract

Here we introduce a new NASICON-type Na3VSc(PO4)3 positive electrode material for Na-ion batteries demonstrating reversible (de)intercalation of 3 Na cations per formula unit within a wide voltage range with complex voltage-composition dependence. The total electrochemical capacity of the material is 170 mAh g-1 that corresponds to the complete three-electron V2+/V3+/V4+/V5+ process. All the (de)sodiation stages follow a predominantly solid-solution mechanism, as shown by operando X-ray powder diffraction. The oxidation of vanadium up to +5 upon the charge of Na3VSc(PO4)3 to 4.5 V vs Na/Na+ causes the significant transformation of the unit cell. According to ex situ Fourier-transformed infrared spectroscopy it is accompanied by the increasing distortion of the vanadium coordination environment and shortening of the vanadium-oxygen bonds. This leads to the irreversible character of the charge-discharge curve, and the initial structure can be restored after the strong overdischarge to ≈1.5 V vs Na/Na+

Original languageEnglish
Article number110550
JournalJournal of the Electrochemical Society
Volume168
Issue number11
DOIs
Publication statusPublished - Nov 2021

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