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Tailoring the Reaction Heterogeneity for Robust Li-Rich Cathodes
Yuanyuan Liu1, Saichao Li1, Jiantao Li2
1State Key Lab of Physical Chemistry of Solid Surface, Fujian Key Laboratory of Surface and Interface Engineering for High Performance Materials, College of Materials, Xiamen University, Xiamen, 361005, China.
Advanced Materials (Deerfield Beach, Fla.)
|October 14, 2025
Summary
Engineered compositional gradients in lithium-rich manganese-based layered oxide (LLO) cathodes improve stability by controlling particle-level reactions. This strategy enhances electrochemical performance and reduces degradation for robust battery applications.
Area of Science:
- Materials Science
- Electrochemistry
- Energy Storage
Background:
- Lithium-rich manganese-based layered oxides (LLO) are promising cathode materials for high-energy batteries.
- However, their practical application is limited by capacity and voltage degradation due to oxygen release and phase transitions.
Purpose of the Study:
- To engineer reaction heterogeneity in LLO cathodes via compositional gradient design.
- To couple Li+ transport kinetics and anion redox activity for improved electrochemical performance.
Main Methods:
- Compositional gradient design within individual cathode particles.
- Analysis of spatially resolved electrochemical divergence (reaction heterogeneity).
- Investigating the impact of Co/Mn concentration gradients on phase distribution and structural ordering.
Main Results:
- A Co/Mn concentration gradient creates surface-bulk reaction heterogeneity.
- A Li2MnO3-poor, Co-enriched surface mitigates oxygen loss and enhances kinetics.
- A Li2MnO3-enriched core provides high capacity and stability.
- Achieved 86.0% capacity retention and reduced voltage decay after 500 cycles.
Conclusions:
- Tailoring reaction heterogeneity through compositional gradients is a viable strategy for robust LLO cathodes.
- Enhanced anion redox reversibility, Li+ diffusion, and structural stability contribute to exceptional electrochemical properties.
- This approach offers a valuable method for optimizing LLO cathode chemistry and performance.
