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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 summary is machine-generated.

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.

Keywords:

LiCoO2 lattice O phase transition subsurface structure ultrahigh‐capacity

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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.