Self-Reinforcing Structural-Interfacial Evolution in LiCuFe₂(VO₄)₃ Anodes Enables Durable, High-Capacity Lithium...

Area of Science:

• Materials Science
• Electrochemistry
• Energy Storage

Background:

• Designing high-capacity, durable anodes for lithium-ion batteries (LIBs) is challenging due to structural degradation and slow interfacial kinetics.
• Existing anode materials often suffer from capacity fade over extended cycling.
• Novel material design is crucial for advancing LIB technology.

Purpose of the Study:

• To engineer a novel polycationic vanadate-based compound, LiCuFe2(VO4)3, for high-performance LIB anodes.
• To investigate the coupled mechanism of electrochemical lattice reorganization and self-adaptive interface modulation.
• To address structural degradation and interfacial kinetic issues in LIB anodes.

Main Methods:

• Synthesis and electrochemical testing of LiCuFe2(VO4)3 as an anode material.
• Synchrotron radiation X-ray diffraction (SR-XRD) for in-situ structural analysis during cycling.
• First-principles calculations to elucidate reaction mechanisms and interfacial behavior.

Main Results:

• Exceptional cycling stability: 1178 mAh g−1 retained after 1000 cycles at 0.5 A g−1, with capacity elevation.
• Electrochemical lattice reorganization: Precipitation of Cu nanoparticles and formation of Fe3O4.
• Self-adaptive interface modulation: Dynamic electrolyte translation forming a polymer gel-like film, alleviating stress and enabling surface-dominated storage.

Conclusions:

• LiCuFe2(VO4)3 demonstrates a promising dual-regulation mechanism for enhanced anode performance.
• The material exhibits superior cycling stability and capacity retention, overcoming key LIB challenges.
• This work presents an electrochemically induced optimization paradigm for next-generation LIB anode materials.