Li−N Interaction Induced Deep Eutectic Gel Polymer Electrolyte for High Performance Lithium‐Metal Batteries

As emerging eutectic mixtures, deep eutectic electrolytes (DEEs) show unique properties for Li‐metal batteries (LMBs). However, the limited choice and inferior electrode compatibility hinder their further development in LMBs. Herein, we report a new 1,2‐dimethylimidazole (DMIm)‐based deep eutectic g...

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Published in:Angewandte Chemie 2022-08, Vol.134 (31), p.n/a
Main Authors: Pei, Xiaopeng, Li, Yiju, Ou, Ting, Liang, Xuechen, Yang, Yun, Jia, Erna, Tan, Ying, Guo, Shaojun
Format: Article
Language:English
Subjects:
1,2-Dimethylimidazole
Batteries
Chemistry
Deep Eutectic Electrolytes
Difluorides
Electrolytes
Eutectic Gel Electrolytes
Eutectics
Flammability
Interface stability
Ion currents
Ions
Lithium
Lithium ions
Lithium-Metal Batteries
Oxidation
Polymers
Polyvinylidene Difluoride
Polyvinylidene fluorides
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Summary:As emerging eutectic mixtures, deep eutectic electrolytes (DEEs) show unique properties for Li‐metal batteries (LMBs). However, the limited choice and inferior electrode compatibility hinder their further development in LMBs. Herein, we report a new 1,2‐dimethylimidazole (DMIm)‐based deep eutectic gel polymer electrolyte induced by Li−N interaction. We demonstrate that incorporating electron‐withdrawing polyvinylidene difluoride (PVDF) polymer into the DMIm‐based DEE changes the coordination environment of Li+ ions, leading to a high transference number of Li+ ions (0.65) and superior interface stability between the electrolyte and Li anode. The deep eutectic gel polymer electrolyte exhibits excellent non‐flammability, high ionic conductivity (1.67 mS cm−1 at 30 °C), and high oxidation voltage (up to 4.35 V vs. Li/Li+). The Li||LFP cell based on the newly developed deep eutectic gel polymer electrolyte can achieve superior long‐term cycling stability at a wide range of rates. A new Li−N interaction induced 1,2‐dimethylimidazole (DMIm)‐based deep eutectic gel polymer electrolyte is reported. The electron‐donating DMIm dissociates LiTFSI well to form a deep eutectic electrolyte (DEE). The incorporation of polyvinylidene difluoride (PVDF) further changes the coordination environment of the Li+ ions. This kind of gel polymer electrolyte exhibits high ionic conductivity and electrochemical stability and enables the excellent long‐term cycling performance for Li/LFP cells.
ISSN:0044-8249
1521-3757
DOI:10.1002/ange.202205075