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Probing the microstructural changes in Li-rich layered oxides induced by over-lithiation
Yifan Wang1, Xiaoxia Yang2,3, Xinyue Zhai2
1Key Lab of Fuel Cell Technology of Guangdong Province, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510641, Guangdong, China. jqhusc@scut.edu.cn.
Chemical Communications (Cambridge, England)
|December 10, 2025
Summary
Li-rich manganese-based layered oxides (LRMO) exhibit high capacity but degrade quickly. Strain accumulation during over-lithiation, not lattice changes, causes this capacity fading in LRMO cathode materials.
Area of Science:
- Materials Science
- Electrochemistry
- Solid-State Chemistry
Background:
- Li-rich manganese-based layered oxides (LRMO) are promising cathode materials for high-energy-density lithium-ion batteries.
- LRMOs offer high specific capacity (~400 mAh g⁻¹) but suffer from significant capacity degradation during cycling.
- Understanding the structural evolution is crucial for improving LRMO performance.
Purpose of the Study:
- To investigate the crystal structure evolution and strain variations in Li₁₂Ni₀₂Mn₀₆O₂ cathode materials.
- To correlate structural changes with capacity fading mechanisms in LRMOs.
- To identify the primary cause of degradation in LRMO cathode materials.
Main Methods:
- Synchrotron X-ray diffraction (sXRD) was employed to analyze crystal structure.
- Materials were studied over a wide voltage range (1.0-4.8 V).
- Microstrain, lattice parameters, and unit-cell volume were systematically evaluated.
Main Results:
- Significant microstrain changes were observed as voltage decreased below 2.0 V.
- Lattice parameters and unit-cell volume showed relatively small variations.
- Capacity fading correlated strongly with strain accumulation during over-lithiation.
Conclusions:
- The primary cause of rapid capacity fading in LRMOs is the accumulation of strain.
- Over-lithiation leads to detrimental strain build-up, impacting long-term cyclability.
- Targeting strain mitigation strategies is essential for enhancing LRMO cathode stability.
