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The Relationship between Ionic Conductivity and Solvation Structures of Localized High-Concentration Fluorinated Electrolytes for Lithium-Ion Batteries

Journal Article · · Journal of Physical Chemistry Letters
Localized high concentration electrolyte (LHCE) combines a diluent with high concentration electrolyte (HCE), offering promising properties. The ions, solvent, and diluent interact to form a complex heterogenous liquid structure, where high salt concentration clusters are embedded in diluent. Optimizing LHCE for desired electrolyte properties like high ionic conductivity, low viscosity, effective solid electrolyte interphase (SEI) formability, within the vast chemical and compositional design space requires deeper understanding and theoretical guidance. For this work, we investigated the structures and conductivity of LHCEs based on a fluorinated solvent with two different diluents at varying concentrations. The 2,2,3,3-tetrafluoropropyl trifluoroacetate (TFPTFA) enters the solvation cluster due to its stronger Li-ion interactions, whereas 1,1,2,2-tetrafuoroethyl 2,2,2-trifuoroethyl ether (TFETFE) enters only at extremely high diluent concentrations. The ionic conductivity increases with decreasing diluent concentrations, with a slope change during cluster percolation. Overall, TFETFE demonstrates higher effectiveness than TFPTFA, forming higher local salt concentration clusters, and resulting in higher ionic conductivity.
Research Organization:
Brown Univ., Providence, RI (United States); Stony Brook Univ., NY (United States); Univ. of California, San Diego, CA (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)
Grant/Contract Number:
EE0009643; EE0009648
Other Award/Contract Number:
2234683
OSTI ID:
3024082
Alternate ID(s):
OSTI ID: 2418088
Journal Information:
Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 34 Vol. 14; ISSN 1948-7185
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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