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Tailoring chemical composition of solid electrolyte interphase by selective dissolution for long-life micron-sized
Yi-Fan Tian1,2, Shuang-Jie Tan1, Chunpeng Yang3
1CAS Key Laboratory of Molecular Nanostructure and Nanotechnology CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry Chinese Academy of Sciences (CAS), 100190, Beijing, P. R. China.
Nature Communications
|November 9, 2023
Summary
Researchers developed a solvent-induced strategy to stabilize micron-sized silicon anodes for batteries. This method enhances the solid electrolyte interphase (SEI) by selectively dissolving weak components, improving cycling stability and battery performance.
Area of Science:
- Materials Science
- Electrochemistry
- Battery Technology
Background:
- Micron-sized silicon anodes offer higher capacity than graphite but suffer from severe volume expansion during lithiation.
- Existing solid electrolyte interphases (SEIs) lack the mechanical stability to accommodate this expansion, limiting silicon anode performance.
- Developing robust SEIs is crucial for realizing the potential of silicon anodes in high-energy batteries.
Purpose of the Study:
- To develop a novel strategy for in situ regulation of SEI mechanical properties.
- To enhance the cycling stability and performance of micron-sized silicon anodes.
- To establish a guideline for designing electrolytes to stabilize alloying-type anodes.
Main Methods:
- Introduced a high-donor-number solvent, gamma-butyrolactone, into conventional electrolytes.
- Utilized a solvent-induced selective dissolution strategy to modify the SEI composition.
- Investigated the effect of solvent donor number on SEI properties and cycling performance.
- Tested raw and carbon-coated micron-sized silicon anodes in electrochemical cells.
Main Results:
- Selective dissolution of low-modulus SEI components (e.g., Li alkyl carbonates) was achieved, leaving a robust SEI (LiF and polycarbonates).
- Raw micron-sized Si anodes retained 87.5% capacity after 100 cycles at 0.5 C.
- Carbon-coated micron-sized Si anodes achieved over 300 cycles.
- A Si||NCM battery demonstrated 83.7% capacity retention after 150 cycles.
Conclusions:
- Solvent-induced selective dissolution is an effective strategy for tailoring SEI properties and enhancing silicon anode stability.
- The donor number of solvents directly correlates with SEI modification and improved cycling life.
- Designing high-donor-number electrolytes is a promising approach for stabilizing volume-changing anodes in high-energy rechargeable batteries.

