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Locally Concentrated Ionic Liquid Electrolytes Enabling Low‐Temperature Lithium Metal Batteries

Liu, Xu 1,2; Mariani, Alessandro; Diemant, Thomas 1,2; Dong, Xu 1,2; Su, Po-Hua 1,2; Passerini, Stefano 2,3
1 Karlsruher Institut für Technologie (KIT)
2 Center for Electrochemical Energy Storage Ulm & Karlsruhe (CELEST), Karlsruher Institut für Technologie (KIT)
3 Helmholtz-Institut Ulm (HIU), Karlsruher Institut für Technologie (KIT)

Abstract:

Lithium metal is a promising anode material for next-generation high-energy-density batteries but suffers from low stripping/plating Coulombic efficiency and dendritic growth particularly at sub-zero temperatures. Herein, a poorly-flammable, locally concentrated ionic liquid electrolyte with a wide liquidus range extending well below 0 °C is proposed for low-temperature lithium metal batteries. Its all-anion Li$^+$ solvation and phase-nano-segregation solution structure are sustained at low temperatures, which, together with a solid electrolyte interphase rich in inorganic compounds, enable dendrite-free operation of lithium metal anodes at −20 °C and 0.5 mA cm$^{−2}$, with a Coulombic efficiency of 98.9 %. As a result, lithium metal batteries coupling thin lithium metal anodes (4 mAh cm$^{−2}$) and high-loading LiNi$_{0.8}$Co$_{0.15}$Al$_{0.05}$O$_2$ cathodes (10 mg $^{−2}$) retain 70 % of the initial capacity after 100 cycles at −20 °C. These results, as a proof of concept, demonstrate the applicability of locally concentrated ionic liquid electrolytes for low-temperature lithium metal batteries.


Verlagsausgabe §
DOI: 10.5445/IR/1000160565
Veröffentlicht am 21.12.2023
Originalveröffentlichung
DOI: 10.1002/anie.202305840
Scopus
Zitationen: 17
Web of Science
Zitationen: 13
Dimensions
Zitationen: 18
Cover der Publikation
Zugehörige Institution(en) am KIT Center for Electrochemical Energy Storage Ulm & Karlsruhe (CELEST)
Helmholtz-Institut Ulm (HIU)
Publikationstyp Zeitschriftenaufsatz
Publikationsjahr 2023
Sprache Englisch
Identifikator ISSN: 1433-7851, 0570-0833, 1521-3773
KITopen-ID: 1000160565
HGF-Programm 38.02.01 (POF IV, LK 01) Fundamentals and Materials
Erschienen in Angewandte Chemie - International Edition
Verlag John Wiley and Sons
Band 62
Heft 31
Seiten Art.Nr.: e202305840
Vorab online veröffentlicht am 22.06.2023
Schlagwörter Ionic Liquid Electrolytes, Lithium Metal Anodes, Locally Concentrated Electrolytes, Low Temperature Batteries
Nachgewiesen in Scopus
Web of Science
Dimensions
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