Impact of Fluorine‐Based Lithium Salts on SEI for All‐Solid‐State PEO‐Based Lithium Metal Batteries

Author:

Li Jiajia12ORCID,Hu Haiman1,Fang Wenhao2,Ding Junwei1,Yuan Du3,Luo Shuangjiang2,Zhang Haitao2,Ji Xiaoyan1ORCID

Affiliation:

1. Energy Engineering Division of Energy Science Luleå University of Technology Luleå 97187 Sweden

2. CAS Key Laboratory of Green Process and Engineering Beijing Key Laboratory of Ionic Liquids Clean Process Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 China

3. College of Materials Science and Engineering Changsha University of Science and Technology 960, 2nd Section, Wanjiali RD (S) Changsha Hunan 410004 China

Abstract

AbstractLiF‐rich solid‐electrolyte‐interphase (SEI) can suppress the formation of lithium dendrites and promote the reversible operation of lithium metal batteries. Regulating the composition of naturally formed SEI is an effective strategy, while understanding the impact and role of fluorine (F)‐based Li‐salts on the SEI characteristics is unavailable. Herein, LiFSI, LiTFSI, and LiPFSI are selected to prepare solid polymer electrolytes (SPEs) with poly(ethylene oxide) and polyimide, investigating the effects of molecular size, F contents and chemical structures (F‐connecting bonds) of Li‐salts and revealing the formation of LiF in the SEI. It is shown that the F‐connecting bond is more significant than the molecular size and F element contents, and thus the performances of cells using LiPFSI are slightly better than LiTFSI and much better than LiFSI. The SPE containing LiPFSI can generate a high amount of LiF, and SPEs containing LiPFSI and LiTFSI can generate Li3N, while there is no Li3N production in the SEI for the SPE containing LiFSI. The preferential breakage bonds in LiPFSI are related to its position to Li anode, where Li‐metal as the anode is important in forming LiF, and consequently the LiPFSI reduction mechanism is proposed. This study will boost other energy storage systems beyond Li‐ion chemistries.

Funder

Vinnova

National Key Research and Development Program of China

Publisher

Wiley

Subject

Electrochemistry,Condensed Matter Physics,Biomaterials,Electronic, Optical and Magnetic Materials

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