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Insights into Electrolytic Pre-Lithiation: A Thorough Analysis Using Silicon Thin Film Anodes
Lukas Haneke1, Felix Pfeiffer2, Peer Bärmann3
1University of Münster, MEET Battery Research Center, Institute of Physical Chemistry, Corrensstraße 46, 48149, Münster, Germany.
Small (Weinheim an Der Bergstrasse, Germany)
|December 12, 2022
Summary
Electrolytic pre-lithiation using cost-effective LiCl electrolytes enables high-silicon lithium-ion batteries. This method forms a protective solid electrolyte interphase (SEI) on silicon electrodes, improving full-cell capacity retention.
Area of Science:
- Electrochemistry
- Materials Science
- Energy Storage
Background:
- High silicon content negative electrodes are crucial for advanced lithium-ion batteries.
- Pre-lithiation is essential to compensate for the initial lithium loss in silicon anodes.
- Existing pre-lithiation methods can be complex or costly.
Purpose of the Study:
- To demonstrate electrolytic pre-lithiation as a viable method for silicon-based lithium-ion batteries.
- To optimize electrolytes for effective solid electrolyte interphase (SEI) formation on silicon.
- To evaluate the performance and stability of electrolytic pre-lithiation in full cells.
Main Methods:
- Electrolytic pre-lithiation using lithium chloride (LiCl) based electrolytes.
- Electrolyte optimization with boron-containing additives and CO2 for SEI formation.
- Characterization using cyclic voltammetry, X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), and impedance spectroscopy.
- Testing in Si||Li metal cells and NCM111||Si full cells.
Main Results:
- Optimized LiCl electrolytes achieved reversible lithiation with 95-96% Coulombic efficiency in Si||Li metal cells.
- Effective SEI formation on silicon electrodes was confirmed by XPS and cyclic voltammetry.
- Electrolytic pre-lithiation significantly improved capacity retention in NCM111||Si full cells from 54% to 78% after 100 cycles.
- A chlorine shuttle mechanism was identified but did not degrade silicon or SEI.
Conclusions:
- Electrolytic pre-lithiation is a promising technique for high-silicon lithium-ion batteries.
- Cost-efficient LiCl electrolytes can be optimized for stable SEI formation and high performance.
- This method enhances the practical viability of silicon anodes in next-generation energy storage devices.
