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Lithium Pre-Storage Enables High Initial Coulombic Efficiency and Stable Lithium-Enriched Silicon/Graphite Anode
Ying-Jie Gao1,2, Cheng-Hao Cui1,2, Zhi-Kun Huang1,2
1State Key Lab of High Performance Ceramics and Superfine microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Dingxi Road, Shanghai, 200050, P. R. China.
Angewandte Chemie (International Ed. in English)
|April 21, 2024
Summary
This study introduces a stable lithium pre-storage method for silicon anodes, achieving ultra-high initial Coulombic efficiency (ICE) and improved cyclability for better battery performance.
Area of Science:
- Materials Science
- Electrochemistry
- Energy Storage
Background:
- Silicon anodes face challenges with low initial Coulombic efficiency (ICE) and poor cyclability.
- Traditional pre-lithiation reagents lack stability and pose safety risks.
- Developing water-stable, high-ICE prelithiated silicon is crucial for advanced batteries.
Purpose of the Study:
- To develop a stable and effective pre-lithiation method for silicon anodes.
- To enhance the initial Coulombic efficiency (ICE) and cycling stability of silicon-based anodes.
- To create air- and water-stable prelithiated silicon materials.
Main Methods:
- A novel lithium pre-storage methodology using nano-drilled graphite with surficial lithium functional groups.
- High-temperature sintering to form chemical bonds between lithium functional groups on graphite and silicon nanoparticles.
- In situ pre-lithiation of silicon nanoparticles via an O-Li-Si interaction.
Main Results:
- Achieved an ultra-high initial Coulombic efficiency (ICE) of ≥110%.
- Demonstrated excellent air and water stability of the lithium-enriched silicon/graphite material.
- Exhibited a high specific capacity of 620 mAh g⁻¹ and long cycling stability (>400 cycles).
Conclusions:
- The developed lithium pre-storage method offers a promising solution for stable silicon anode pre-lithiation.
- This approach overcomes the limitations of traditional pre-lithiation reagents, enhancing safety and performance.
- The lithium-enriched silicon/graphite material paves the way for next-generation high-performance, stable batteries.

