Stabilizing Multi-Electron NASICON-Na1.5V0.5Nb1.5(PO4)< sub>3 Anode via Structural Modulation for Long-Life Sodium-Ion Batteries
ADVANCED ENERGY MATERIALS(2024)
摘要
Multi-electron NAtrium SuperIonic CONductor (NASICON)-Nb-2(PO4)(3) (N0NbP) is an attractive Na-ion battery anode, owing to its low intercalation voltage (1.4 V vs Na+/Na-0) and high capacity (approximate to 150 mAh g(-1)). However, it suffers from poor capacity retention due to structural degradation. To overcome this issue, extra Na+ ions are introduced at the Na(1) sites, via V3+ substitution, which can act as stabilizing agents to hold lantern units together during cycling, producing NASICON-Na1.5V0.5Nb1.5(PO4)(3) (N1.5VNbP). The N1.5VNbP anode exhibits reversible capacities of approximate to 140 mAh g(-1) at 1.4 V versus Na+/Na-0 through Nb5+/Nb4+/Nb3+ and V3+/V2+ redox activities. The extra Na+ ions in the framework forms a complete solid-solution during Na (de)intercalation and enhances sodium diffusivity, in agreement with first-principles calculations. Further, N1.5VNbP demonstrates extraordinary cycling (89% capacity retention at 5C after 500 cycles) and rate performances (105 mAh g(-1) at 5C). Upon pairing the N1.5VNbP anode with the NASICON-Na3V2(PO4)(3) cathode, the full Na-ion cell delivers a remarkable energy density of 98 Wh kg(-1) (based on the mass of anode and cathode) and retains 80% of its capacity at 5C rate over 1000 cycles. The study opens new possibilities for enhancing the electrochemical performance of NASICON anodes via chemical and structural modulations.
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关键词
multielectron reaction,Na1.5V0.5Nb1.5(PO4)(3),Na-ion batteries,NASICON anode,structural modulation
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