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

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Tuning Li occupancy and local structures for advanced Co-free Ni-rich positive electrodes.

Hang Li^1,2, Hao Liu³, Shunrui Luo⁴

¹School of Advanced Materials, Peking University Shenzhen Graduate School, Shenzhen, China. 2206393335@pku.edu.cn.

Nature Communications

|March 5, 2025

Summary

This study reveals how lithium occupancy impacts the stability of nickel-rich battery electrodes. Tuning lithium distribution improves electrode durability and battery performance.

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Area of Science:

Materials Science
Electrochemistry
Battery Technology

Background:

Nickel-rich positive electrodes are critical for high-energy lithium-ion batteries.
Structural evolution and surface reactivity are key research areas.
The role of lithium occupancy in electro-chemomechanical stability remains underexplored due to challenges in Li determination.

Purpose of the Study:

To comprehensively analyze the influence of lithium occupancy on structural domains and stability in Ni-rich positive electrodes.
To introduce and evaluate a Li-regulation strategy for tuning these domains.
To investigate the impact of Li distribution on redox mechanisms and overall battery performance.

Main Methods:

Utilized Li-sensitive characterization techniques for detailed Li occupancy analysis.
Employed a Li-regulation strategy to control the ratio of different structural domains.
Designed and tested specific Ni-rich positive electrodes with tuned Li distribution.

Main Results:

Identified distinct Li occupancies and associated structural domains (e.g., Ni/Li exchange, Li$_{a}$XO$_{b}$, Li/Mn/X(Ni) ordering).
Demonstrated effective tuning of domain ratios via the Li-regulation strategy.
Achieved notable improvements in battery cyclability for designed electrodes.

Conclusions:

Lithium occupancy is a critical, previously overlooked factor in Ni-rich electrode stability.
Tuning Li distribution significantly enhances electrode durability and electrochemical performance.
This approach provides new insights for designing advanced, long-lasting Ni-rich positive electrodes.