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Engineering a Dynamic Solvent-Phobic Liquid Electrolyte Interphase for Long-Life Lithium Metal Batteries
Qi Kang1, Yong Li2, Zechao Zhuang3
1Department of Polymer Science and Engineering, Shanghai Key Laboratory of Electrical Insulation and Thermal Ageing, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China.
Advanced Materials (Deerfield Beach, Fla.)
|January 25, 2024
Summary
This study introduces a novel solvent-phobic dynamic liquid electrolyte interphase (DLEI) for lithium metal batteries (LMBs). The DLEI enhances cycling stability and capacity retention in carbonate electrolytes by forming a stable, salt-derived solid electrolyte interphase (SEI).
Area of Science:
- Materials Science
- Electrochemistry
- Energy Storage
Background:
- Conventional solid electrolyte interphases (SEIs) in lithium metal batteries (LMBs) suffer from heterogeneity and poor mechanical stability, leading to irreversible lithium and electrolyte loss.
- This instability limits the practical application and cycling performance of LMBs, particularly those using carbonate electrolytes.
Purpose of the Study:
- To develop a novel dynamic liquid electrolyte interphase (DLEI) that stabilizes the lithium metal-electrolyte interface.
- To induce the formation of a robust, salt-derived SEI that mitigates side reactions and improves battery longevity.
Main Methods:
- A solvent-phobic DLEI, Li-PFbTHF (perfluoro-butyltetrahydrofuran), was designed with C-F-rich groups to selectively transport salt and form a salt-derived SEI.
- In situ electrochemical impedance spectroscopy and Ab-initio molecular dynamics were employed to analyze interface stability.
- Electrochemical performance was evaluated using LiFePO4||Li half-cells and LiFePO4/Li full cells, along with a 0.55 Ah pouch cell.
Main Results:
- The solvent-phobic DLEI effectively reduced side reactions with carbonate solvents and humid air, forming a LiF/Li3PO4-rich SEI.
- Interface stabilization was confirmed by electrochemical impedance spectroscopy and molecular dynamics simulations.
- LiFePO4||Li-PFbTHF cells showed 80.4% capacity retention after 1000 cycles at 1.0 C, and full cells achieved 90.2% retention after 550 cycles.
- A 0.55 Ah pouch cell demonstrated stable cycling with an energy density of 252.0 Wh kg-1.
Conclusions:
- The proposed solvent-phobic DLEI strategy effectively controls salt-derived SEI formation, significantly enhancing the cycling performance of carbonate-based LMBs.
- This approach offers a promising pathway for developing stable and high-performance lithium metal batteries.
