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Locally Concentrated Ionic Liquid Electrolyte with Partially Solvating Diluent for Lithium/Sulfurized Polyacrylonitrile Batteries

Liu, Xu 1; Diemant, Thomas 1; Mariani, Alessandro 1; Dong, Xu 1; Di Pietro, Maria Enrica; Mele, Andrea; Passerini, Stefano 1
1 Helmholtz-Institut Ulm (HIU), Karlsruher Institut für Technologie (KIT)

Abstract:

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.


Verlagsausgabe §
DOI: 10.5445/IR/1000153036
Veröffentlicht am 25.11.2022
Originalveröffentlichung
DOI: 10.1002/adma.202207155
Scopus
Zitationen: 15
Web of Science
Zitationen: 7
Dimensions
Zitationen: 18
Cover der Publikation
Zugehörige Institution(en) am KIT Helmholtz-Institut Ulm (HIU)
Publikationstyp Zeitschriftenaufsatz
Publikationsjahr 2022
Sprache Englisch
Identifikator ISSN: 0935-9648, 1521-4095
KITopen-ID: 1000153036
HGF-Programm 38.02.01 (POF IV, LK 01) Fundamentals and Materials
Erschienen in Advanced Materials
Verlag John Wiley and Sons
Band 34
Heft 49
Seiten Art.-Nr.: 2207155
Vorab online veröffentlicht am 31.10.2022
Schlagwörter ionic liquids, lithium-metal anodes, locally concentrated electrolytes, sulfurized polyacrylonitrile
Nachgewiesen in Dimensions
Web of Science
Scopus
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