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Ligand-channel-enabled ultrafast Li-ion conduction

Journal Article · · Nature (London)
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  1. Zhejiang University, Hangzhou (China)
  2. Brookhaven National Laboratory (BNL), Upton, NY (United States)
  3. Chinese Academy of Sciences (CAS), Beijing (China); University of the Chinese Academy of Sciences, Beijing (China)
  4. University of Maryland, College Park, MD (United States)
  5. Zhejiang University, Hangzhou (China); Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang Province, Hangzhou (China)
+ Show Author Affiliations
Li-ion batteries (LIBs) for electric vehicles and aviation demand high energy density, fast charging and a wide operating temperature range, which are virtually impossible because they require electrolytes to simultaneously have high ionic conductivity, low solvation energy and low melting point and form an anion-derived inorganic interphase. We report guidelines for designing such electrolytes by using small-sized solvents with low solvation energy. The tiny solvent in the secondary solvation sheath pulls out the Li+ in the primary solvation sheath to form a fast ion-conduction ligand channel to enhance Li+ transport, while the small-sized solvent with low solvation energy also allows the anion to enter the first Li+ solvation shell to form an inorganic-rich interphase. The electrolyte-design concept is demonstrated by using fluoroacetonitrile (FAN) solvent. The electrolyte of 1.3 M lithium bis(fluorosulfonyl)imide (LiFSI) in FAN exhibits ultrahigh ionic conductivity of 40.3 mS cm-1 at 25 °C and 11.9 mS cm-1 even at -70 °C, thus enabling 4.5-V graphite||LiNi0.8Mn0.1Co0.1O2 pouch cells (1.2 Ah, 2.85 mAh cm-2) to achieve high reversibility (0.62 Ah) when the cells are charged and discharged even at -65 °C. The electrolyte with small-sized solvents enables LIBs to simultaneously achieve high energy density, fast charging and a wide operating temperature range, which is unattainable for the current electrolyte design but is highly desired for extreme LIBs. This mechanism is generalizable and can be expanded to other metal-ion battery electrolytes.
Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
Central Universities; National Natural Science Foundation of China; Natural Science Foundation of Zhejiang Province; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)
Grant/Contract Number:
SC0012704
OSTI ID:
2336570
Report Number(s):
BNL--225461-2024-JAAM
Journal Information:
Nature (London), Journal Name: Nature (London) Journal Issue: 8002 Vol. 627; ISSN 0028-0836
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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