Abstract Lithium (Li) metal batteries offer high energy densities but suffer from uncontrolled lithium deposition, causing serious dendrite growth and volume fluctuation. Tailorable Li nucleation and uniform early‐stage plating are essential for homogenous Li deposition. Herein, insertion type Li 3 VO 4 is first demonstrated as efficient lithiophilic sites trapping Li + ions for homogenous nucleation. By homogenizing the distribution of electric field and ions flux via an ingenious architecture design with Li 3 VO 4 nanodots grown on the carbon fibers (LVO@CNFs), leveling Li metal deposition after nucleation is also realized. These, together, result in smooth and dendrite‐free Li deposition on the LVO@CNFs via a trapping‐and‐leveling model, giving rise to unprecedented performance (highly stable Li plating/stripping exceeding 2500 h at 2 mA cm −2 under 3 mA h cm −2 capacity, high‐capacity retention of 82.5% over 500 cycles in a Li@LVO@CNFs//LiFePO 4 battery). The successful design of Li metal deposition host via insertion‐type Li 3 VO 4 may pave a new way for long lifespan Li metal batteries.
Oxides based on vanadium redox couple, such as orthorhombic Li3VO4, has drawn great attentions due to its high theoretical capacity and moderate operating voltage. However, the rate property is largely hindered by the slow interfacial dynamics of Li3VO4. Here we synthesized the lotus stem-like Li3VO4 wrapped in N-doped carbon fibers (Li3VO4/C NF) stemmed from the chemical lithiation of V2O3/C NF. The knobbly Li3VO4 rooted in the interconnected carbon fibers provides abundant active sites and well-developed conductive networks. Thus, this anode delivers high specific capacity of 558.9 mAh g-1 at 0.2 A g-1 and excellent rate capacity of 419 mAh g-1 at 2 A g-1 sustaining 900 cycles with an average potential of 0.7 V vs. Li+/Li. Furthermore, the kinetic analysis reveals that the pseudocapacitance dominants the lithium storage process and the favorable interfacial ion and electronic transport is responsible for the enhanced rate performance. The full cell (Li3VO4/C NF||LiFePO4) also shows a competitive performance for commercialization. This work boosts the development of vanadium-based anode materials with desired electrochemical properties meeting devices requirements.
A concise electrospraying approach was developed to synthesize novel Li 3 VO 4 /C honeycombs comprised of Li 3 VO 4 @C nanoparticles, which show an unprecedented high-rate lifespan, demonstrating great potential toward high-power applications.
Abstract Na 3 V 2 O 2 (PO 4 ) 2 F (NVOPF) as an attractive electrode material has received much attention based on the one‐electron reaction of V 4+ /V 5+ . However, the electrochemical reactions involving lower vanadium valences were not investigated till now. Herein, a composite of graphene decorated nanosheet‐assembled NVOPF microflowers (NVOPF/G) was synthesized and the multi‐electron reaction of NVOPF/G was conducted by controlling the operation voltage windows. The reaction mechanism, structural changes, and vanadium valences during the insertion/extraction of Li ions (from 2 to 6) were elucidated clearly by in‐situ X‐ray diffraction and ex‐situ X‐ray photoelectron spectroscopy. Theoretical computations also revealed the Li‐ion locations in the structure of NaV 2 O 2 (PO 4 ) 2 F. Due to the additional redox couple of V 3+ /V 4+ , NVOPF/G displayed a much higher initial capacity of 183.3 mAh g −1 in the wider voltage window of 1.0–4.8 V than that of 2.5–4.8 V (129.3 mAh g −1 ). Moreover, excellent Li‐storage performance of NVOPF/G at a lower voltage (≤2.5 V) with the active reaction of V 2+ /V 3+ /V 4+ was obtained for the first time, demonstrating the high potential of NVOPF/G as an anode material for Li ion storage.
Li3VO4 (LVO) is one of the most promising anode materials for lithium-ion batteries, however, its low electronic conductivity and initial Columbic efficiency pose significant challenges for further applications. To address...
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