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Synergistic Anionic and Cationic Codoping Enables High-Performance LiNi0.5Mn1.5O4 Cathodes
Lingbing Wu1,2, Shan Wang2, Ruida Zhao2
1Electronic Materials Research Laboratory, Key Laboratory of the Ministry of Education, School of Future Technology, and the National Innovation Platform (Center) for Industry Education Integration of Energy Storage Technology, Xi'an Jiaotong University, Xi'an 710049, China.
ACS Applied Materials & Interfaces
|June 8, 2026
Summary
This study introduces a novel cobalt-free cathode material, LiNi0.47Cu0.01Al0.01Mn1.47Ti0.01V0.01O4-xFx (CATVF), which significantly enhances lithium-ion diffusion and suppresses manganese dissolution for better battery performance.
Area of Science:
- Materials Science
- Electrochemistry
- Solid-State Chemistry
Background:
- LiNi0.5Mn1.5O4 is a promising cobalt-free cathode material for lithium-ion batteries, offering high voltage and energy density.
- Manganese dissolution is a major challenge limiting the commercial application of LiNi0.5Mn1.5O4.
- Developing strategies to overcome manganese dissolution is crucial for advancing high-performance cathode materials.
Purpose of the Study:
- To synthesize a novel cobalt-free cathode material, LiNi0.47Cu0.01Al0.01Mn1.47Ti0.01V0.01O4-xFx (CATVF), using anionic and cationic codoping.
- To investigate the effects of fluorine doping on the material's structure, electrochemical properties, and stability.
- To enhance the lithium-ion diffusion coefficient and mitigate manganese dissolution in spinel cathode materials.
Main Methods:
- Anionic and cationic codoping strategy to synthesize LiNi0.47Cu0.01Al0.01Mn1.47Ti0.01V0.01O4-xFx (CATVF).
- X-ray Photoelectron Spectroscopy (XPS) to analyze the electronic structure and bonding environment.
- Scanning Electron Microscopy (SEM) to study the material's morphology and crystal plane growth.
- Electrochemical testing to evaluate discharge capacity, rate capability, and cycling stability.
Main Results:
- Fluorine doping (F-) strengthens M-F bonds, promotes Mn4+ reduction to Mn3+, and increases ionic disorder.
- F- doping facilitates (110) plane growth and reduces the proportion of (111) planes, influencing material structure.
- The lithium-ion diffusion coefficient was enhanced by four orders of magnitude.
- CATVF-0.01F exhibited a discharge specific capacity of 101.9 mAh g-1 at 30 C and ~90% capacity retention after 300 cycles at 1 C.
- Significant inhibition of manganese dissolution was observed.
Conclusions:
- Anionic and cationic codoping with fluorine is an effective strategy for enhancing the performance of spinel cathode materials.
- The developed CATVF material demonstrates improved lithium-ion diffusion and stability, addressing key limitations of cobalt-free cathodes.
- This approach provides a viable pathway for designing high-performance, cobalt-free cathode materials for next-generation batteries.
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