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Mitigating Surface Irreversible Layer-To-Spinel Phase Transition for Stable and Ultrahigh-Capacity LiCoO2 Cathodes
Haocong Yi1, Wenguang Zhao1, Yutong Lin2
1School of Advanced Materials, Peking University Shenzhen Graduate School, Shenzhen, 518055, China.
Small (Weinheim an Der Bergstrasse, Germany)
|October 31, 2025
Summary
This study introduces dual-optimized lithium cobalt oxide (LCO) cathodes with surface and subsurface modifications. This approach enhances stability and unlocks ultrahigh capacity for advanced battery applications.
Area of Science:
- Materials Science
- Electrochemistry
- Energy Storage
Background:
- Ultrahigh-capacity lithium cobalt oxide (LCO) cathodes face challenges due to surface structure collapse.
- This hinders their practical application in high-performance energy storage devices.
Purpose of the Study:
- To develop a dual-optimized LCO (D-LCO) structure for enhanced stability and capacity.
- To investigate the role of coordinated subsurface and surface modifications in stabilizing LCO cathodes.
Main Methods:
- Fabrication of D-LCO with a surface rocksalt (RS) phase and a subsurface layered phase.
- Incorporation of Al/F doping in the subsurface region to suppress ion migration.
- Electrochemical testing to evaluate capacity, cycling stability, and voltage performance.
Main Results:
- D-LCO achieved an ultrahigh capacity of 236 mAh g⁻¹ at 4.6 V versus Li⁺/Li.
- Demonstrated excellent cycling stability: 90.3% retention after 200 cycles at 1 C and 81.2% after 1000 cycles at 4 C.
- Subsurface Al/F doping effectively suppressed lattice oxygen migration and prevented undesirable phase transitions.
Conclusions:
- Coordinated subsurface and surface stabilization is crucial for unlocking the full potential of layered oxide cathodes.
- The D-LCO strategy provides a pathway for developing next-generation high-energy-density batteries.
- This research addresses critical limitations in LCO cathode technology for energy storage.
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