Journal
ENERGY STORAGE MATERIALS
Volume 35, Issue -, Pages 192-202Publisher
ELSEVIER
DOI: 10.1016/j.ensm.2020.11.010
Keywords
Sodium-deficient NASICON cathode; Single-phase mechanism; In situ X-ray diffraction; Na-23 solid-state nuclear magnetic resonance; DFT calculation
Funding
- National Natural Science Foundation of China [2197040727]
- Fundamental Research Funds for the Central Universities
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The new material exhibits high initial discharge capacity and outstanding rate capability and cycle life, attributed to its small volume change and single-phase mechanism. Experimental data and computational methods reveal the mechanism of sodium extraction and diffusion kinetics. These findings contribute to enhancing the electrochemical performance of sodium-ion batteries.
Sodium-ion battery technology is one of the best alternative candidates to the lithium analogue due to the low cost and the abundance of sodium. Extensive research effort is dedicated to the development of low-cost and highperformance cathodes. Here, a new sodium-deficient NASICON material Na-3.41 0.59FeV(PO4)(3) pound is synthesized by a simple sol-gel method. This new material delivers high initial discharge capacity of 170 mAh g(-1) in the voltage range of 1.5-4.4 V vs. Na+/Na, originating from the intercalation of about 3 Na+ per formula unit. Furthermore, when cycled in the range of 2.0-3.8 V vs. Na+/Na, excellent rate capability and outstanding cycle life are obtained. The remarkable electrochemical performances are attributed to the small volume change (2.36 %) during the sodium extraction through a single-phase mechanism proved by in situ X-ray diffraction (XRD). Refined XRD and 23Na solid-state Nuclear Magnetic Resonance (NMR) combined with Density functional theory (DFT) calculations reveal that the sodium extraction during charge process occurs preferably from Na2 sites. Moreover, this new cathode exhibits high sodium diffusion kinetics confirmed by Galvanostatic Intermittent Titration Technique (GITT). These findings highlight the beneficial use of non-stoichiometry in electrodes for batteries and provide rational design of high-performance cathode materials for sodium-ion batteries.
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