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Characterization of Electrode Materials for Lithium Ion and Sodium Ion Batteries Using Synchrotron Radiation Techniques

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Prolong cycle-life by interlayer doping and vacancy coupling engineering in Li-rich oxide cathodes.

Wang Ke¹, Fu-Da Yu², Yun-Shan Jiang¹

¹MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, State Key Laboratory of Space Power-Sources, Harbin Institute of Technology, Harbin 150001, China.

Journal of Colloid and Interface Science

|June 6, 2025

Summary

Researchers developed interlayer transition metal (TM)-vacancy coupling defects to enhance Li-rich layered oxides (LLOs). This strategy significantly improves cycle-life and capacity retention in LLO cathodes for batteries.

Keywords:

Interlayer TM(Li)-V(TM) coupling defects Li-rich layered oxide Lithium-ion batteries Structure degradation

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Area of Science:

Materials Science
Electrochemistry
Solid-State Chemistry

Background:

Li-rich layered oxides (LLOs) offer high capacity via oxygen anionic redox but suffer from rapid degradation.
Degradation is linked to internal strain, oxygen redox instability, and structural damage, limiting cycle-life.
Previous modifications focused on individual defect types, inspiring combined defect engineering.

Purpose of the Study:

To investigate the effectiveness of constructing interlayer TM-vacancy coupling defects in LLOs.
To enhance the structural stability and electrochemical performance of LLO cathodes.
To achieve both high energy density and long cycle-life in LLO materials.

Main Methods:

Fabrication of LLOs with engineered interlayer TM-vacancy coupling defects.
Electrochemical testing, including cycling stability and voltage decay measurements.
Structural analysis to understand the role of defects in maintaining framework integrity and oxygen redox.

Main Results:

Achieved 85.77% capacity retention and 0.38 mV/cycle voltage decay after 500 cycles at 1C.
Demonstrated that coupled defects maintain the layered framework and occupancy sequence.
Showcased a stable coordination environment for oxygen redox reactions.

Conclusions:

Interlayer TM-vacancy coupling defects effectively suppress layered phase degradation and promote reversible anionic reactions.
This defect engineering strategy provides a pathway to simultaneously achieve high energy density and long cycle-life in LLO cathodes.
The findings highlight the potential of coupling defects for advanced battery materials.