Journal
ADVANCED MATERIALS
Volume 34, Issue 49, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202207155
Keywords
ionic liquids; lithium-metal anodes; locally concentrated electrolytes; sulfurized polyacrylonitrile
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Funding
- China Scholarship Council (CSC)
- German Federal Ministry of Education and Research (BMBF) within the LILLINT project [03XP0225D]
- Helmholtz Association Basic funding
- MSCA EF Master Class 2018
- Projekt DEAL
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This article proposes a new low-flammability locally concentrated ionic liquid electrolyte (LCILE) for Li/sulfurized polyacrylonitrile (SPAN) batteries. The LCILE forms stable electrolyte/electrode interfaces on both the lithium-metal anodes (LMAs) and SPAN cathodes, leading to improved battery performance and cycling stability.
The development of Li/sulfurized polyacrylonitrile (SPAN) batteries requires electrolytes that can form stable electrolyte/electrode interphases simultaneously on lithium-metal anodes (LMAs) and SPAN cathodes. Herein, a low-flammability locally concentrated ionic liquid electrolyte (LCILE) employing monofluorobenzene (mFBn) as the diluent is proposed for Li/SPAN cells. Unlike non-solvating diluents in other LCILEs, mFBn partially solvates Li+, decreasing the coordination between Li+ and bis(fluorosulfonyl)imide (FSI-). In turn, this triggers a more substantial decomposition of FSI- and consequently results in the formation of a solid electrolyte interphase (SEI) rich in inorganic compounds, which enables a remarkable Coulombic efficiency (99.72%) of LMAs. Meanwhile, a protective cathode electrolyte interphase (CEI), derived mainly from FSI- and organic cations, is generated on the SPAN cathodes, preventing the dissolution of polysulfides. Benefiting from the robust interphases simultaneously formed on both the electrodes, a highly stable cycling of Li/SPAN cells for 250 cycles with a capacity retention of 71% is achieved employing the LCILE and only 80% lithium-metal excess.
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