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Journal article : Letter

Imidazolium-based ionic liquid electrolytes for fluoride ion batteries

Abstract:

The fluoride-ion battery (FIB) is a post-lithium anionic battery that utilizes the fluoride-ion shuttle, achieving high theoretical energy densities of up to 1393 Wh L–1 without relying on critical minerals. However, developing liquid electrolytes for FIBs has proven arduous due to the low solubility of fluoride salts and the chemical reactivity of the fluoride ion. By introducing a chemically stable electrolyte based on 1,3-dimethylimidazolium [MMIm] bis(trifluoromethanesulfonyl)imide [TFSI] and tetramethylammonium fluoride (TMAF), we achieve an electrochemical stability window (ESW) of 4.65 V, ionic conductivity of 9.53 mS cm–1, and a solubility of 0.67 m. The origin of this high solubility and the solvation structure were investigated using NMR spectroscopy and neutron total scattering, showing a fluoride solvation driven by strong electrostatic interactions and weak hydrogen bonding without covalent H–F character. This indicates the chemical stability of 1,3-dimethylimidazolium toward the fluoride ion and its potential as an electrolyte for high-voltage FIBs.

 
Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1021/acsenergylett.4c02663

Authors


More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Materials
Role:
Author
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Materials
Role:
Author
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Materials
Role:
Author
ORCID:
0000-0002-3211-2678
More by this author
Role:
Author
ORCID:
0000-0003-0095-5731
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry
Role:
Author
ORCID:
0000-0002-7848-1970


More from this funder
Funder identifier:
https://ror.org/0439y7842
Grant:
EP/R010145/1


Publisher:
American Chemical Society
Journal:
ACS Energy Letters More from this journal
Volume:
9
Issue:
12
Pages:
6104-6108
Place of publication:
United States
Publication date:
2024-11-27
Acceptance date:
2024-11-13
DOI:
EISSN:
2380-8195
Pmid:
39698338


Language:
English
Subtype:
Letter
Pubs id:
2070263
Local pid:
pubs:2070263
Deposit date:
2025-01-04

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