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Intrinsically Nonflammable Ionic Liquid‐Based Localized Highly Concentrated Electrolytes Enable High‐Performance Li‐Metal Batteries
Author(s) -
Wang Zhicheng,
Zhang Fengrui,
Sun Yiyang,
Zheng Lei,
Shen Yanbin,
Fu Daosong,
Li Wanfei,
Pan Anran,
Wang Lei,
Xu Jingjing,
Hu Jianchen,
Wu Xiaodong
Publication year - 2021
Publication title -
advanced energy materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.08
H-Index - 220
eISSN - 1614-6840
pISSN - 1614-6832
DOI - 10.1002/aenm.202003752
Subject(s) - ionic liquid , electrolyte , materials science , electrochemical window , ionic conductivity , chemical engineering , x ray photoelectron spectroscopy , electrochemistry , raman spectroscopy , lithium (medication) , solvent , faraday efficiency , organic chemistry , electrode , chemistry , medicine , physics , optics , engineering , endocrinology , catalysis
Abstract The development of high‐performance Li‐metal batteries (LMBs) requires advanced electrolytes that simultaneously possess high safety, high ionic conductivity, wide electrochemical window, and good ability to suppress Li dendrite growth. Herein an intrinsically nonflammable ionic liquid‐based localized highly concentrated electrolyte (LHCE) composed of lithium bis(fluorosulfonyl)imide (LiFSI) salt, N ‐methyl‐ N ‐propyl‐piperidinium bis(fluorosulfonyl)imide ([PP 13 ][FSI]) as ionic liquid solvent, and 1,1,2,2‐tetrafluoroethyl‐2,2,3,3‐tetrafluoropropylether (HFE) as diluent solvent is designed. The introduction of HFE greatly decreases the viscosity and cost of the pure ionic liquid electrolyte, improves its ionic conductivity, and enhances its ability to wet the separator surface. The Li + solvation structure, Li deposition behavior, and formation of the solid electrolyte interphase (SEI) layer in LHCE are systematically investigated by using Raman spectroscopy, theoretical simulations, scanning electron microscopy, and X‐ray photoelectron spectroscopy. A rational mechanism is suggested for the stable SEI formation and the homogeneous Li deposition behavior. Due to its excellent ability to suppress Li dendrites, the LHCE exhibits a high average Coulombic efficiency (99.4% over 800 cycles in the Cu/Li cell), extremely stable cycling performance (10 mA cm −2 over 5000 cycles in the Li/Li symmetric cell), and excellent cycling performance and rate capability in the LMB systems of LiFePO 4 (LFP)/Li and LFP/Li@Cu.