The development of LiFePO4 (LFP) in high-power energy storage devices is hampered by its slow Li-ion diffusion kinetics. Constructing the composite electrode materials with vanadium substitution is a scientific endeavor to boost LFP’s power capacity. Herein, a series of xLiFePO4·yLi3V2(PO4)3 (xLFP·yLVP) composites were fabricated using a simple spray-drying approach. We propose that 5LFP·LVP is the optimal choice for Li-ion battery promotion, owning to its excellent Li-ion storage capacity (material energy density of 413.6 W·h·kg−1), strong machining capability (compacted density of 1.82 g·cm−3) and lower raw material cost consumption. Furthermore, the 5LFP·LVP||LTO Li-ion pouch cell also presents prominent energy storage capability. After 300 cycles of a constant current test at 400 mA, 75% of the initial capacity (379.1 mA·h) is achieved, with around 100% of Coulombic efficiency. A capacity retention of 60.3% is displayed for the 300th cycle when discharging at 1200 mA, with the capacity fading by 0.15% per cycle. This prototype provides a valid and scientific attempt to accelerate the development of xLFP·yLVP composites in application-oriented Li-ion batteries.
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