Journal
ADVANCED ENERGY MATERIALS
Volume 11, Issue 22, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202100729
Keywords
Na V-3 (2)(PO (4)) (3); Na 4VMn Fe-0 5 (0 5)(PO (4)) (3); NASICON; substitution; synergetic contributions
Categories
Funding
- DNL Cooperation Fund, CAS [DNL201914]
- National Natural Science Foundation of China [U20A20145, 21878195, 51872289, 51672275]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDA21070500]
- National Key Technologies R&D Program, China [2016YFB0901500]
- Innovation Academy for Green Manufacture, CAS
- Beijing Natural Science Foundation [2182074]
- Distinguished Young Foundation of Sichuan Province [2020JDJQ0027]
- Sichuan Science and Technology Project [2019YFH0149]
- Key R&D Project of Sichuan Provincial Department of Science and Technology [2020YFG0471, 2020YFG0022]
- Sichuan Province Science and Technology Achievement Transfer and Transformation Project [21ZHSF0111]
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A novel ternary NASICON-type Na4VMn0.5Fe0.5(PO4)(3)/C cathode is designed with large reversible capacity, high voltage, and good stability. The cathode exhibits excellent rate capacity and cycling durability, outperforming Na4VFe(PO4)(3)/C and Na4VMn(PO4)(3)/C. The synergetic contributions of multimetal ions and facilitated Na+ migration are confirmed, providing new perspectives for high-performance Na-ion batteries.
The Na+ superionic conductor (NASICON)-type Na3V2(PO4)(3) cathodes have attracted extensive interest due to their high structural stability and fast Na+ mobility. However, the substitution of vanadium with low-cost active elements remains imperative due to high cost of vanadium, to further boost its application feasibility. Herein, a novel ternary NASICON-type Na4VMn0.5Fe0.5(PO4)(3)/C cathode is designed, which integrates the advantages of large reversible capacity, high voltage, and good stability. The as-obtained Na4VMn0.5Fe0.5(PO4)(3)/C composite can deliver an excellent rate capacity of 96 m Ah g(-1) at 20 C and decent cycling durability of 94% after 3000 cycles at 20 C, which is superior to that of Na4VFe(PO4)(3)/C and Na4VMn(PO4)(3)/C. The synergetic contributions of multimetal ions and facilitated Na+ migration of the Na4VMn0.5Fe0.5(PO4)(3)/C cathode are confirmed by the first-principles calculations. The processive reduction/oxidation involved in Fe2+/Fe3+, Mn2+/Mn3+, V3+/V4+/V5+ redox couples are also revealed upon the charging/discharging process by ex situ soft X-ray absorption spectroscopy. The reversible structure evolution and small volume change during the electrochemical reaction is demonstrated by in situ X-ray diffraction characterization. The rational design of NASICON-type cathodes by regulating composition with substitution of multimetal ions can provide new perspectives for high-performance Na-ion batteries.
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