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Dynamic cathode-electrolyte interphase structuring by AlF dual surface engineering for exceptional stability of
Hyunsub Shin1, Hojun Moon1, Jaehun Lee1
1Department of Chemistry, College of Natural Sciences, Yeungnam University, Gyeongsan, Gyeongbuk 38541, Republic of Korea.
Journal of Colloid and Interface Science
|November 6, 2025
Summary
High-nickel layered oxides, like NCM811, face challenges in high-voltage lithium-ion batteries. A dual AlF surface modification enhances stability and performance, paving the way for next-generation batteries.
Area of Science:
- Materials Science
- Electrochemistry
- Energy Storage
Background:
- High-nickel layered oxides, such as LiNi₀.₈Co₀.₁Mn₀.₁O₂ (NCM811), are promising cathode materials for high-energy lithium-ion batteries due to their high energy density and lower cobalt content.
- However, their practical application is limited by surface degradation, oxygen release, and lattice instability during high-voltage operation.
Purpose of the Study:
- To develop a dynamic cathode-electrolyte interphase (CEI) engineering strategy for stabilizing high-voltage NCM811 cathodes.
- To investigate the synergistic effects of a dual AlF surface modification on bulk lattice stabilization and interface protection.
Main Methods:
- Synergistic AlF dual surface modification using ammonium fluoride (NH₄F) for fluorination and aluminum oxide (Al₂O₃) nanoshell formation.
- Electrochemical performance testing, including initial discharge capacity and long-term cycling stability at high voltage.
- In-situ and ex-situ characterization techniques such as X-ray diffraction (XRD) and electrochemical impedance spectroscopy (EIS) to analyze structural and interfacial changes.
Main Results:
- The dual-modified NCM811 cathode demonstrated excellent electrochemical performance, with an initial discharge capacity of 227 mAh g⁻¹ at 0.1C and 93.2% capacity retention after 500 cycles at 0.2C.
- The AlF surface modification effectively suppressed lattice distortion and reduced interfacial resistance during high-voltage cycling.
- Formation of a dense, LiF-enriched CEI and a conformal Al₂O₃ nanoshell provided adaptive protection against parasitic reactions and mechanical stress.
Conclusions:
- The proposed dynamic CEI engineering strategy via synergistic AlF dual surface modification significantly enhances the high-voltage stability of Ni-rich cathodes.
- This scalable and cost-effective approach offers a universal platform for improving the commercial viability of NCM811 and similar materials in high-energy lithium-ion batteries.
