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Download fileUnraveling Ion Dynamics and Interactions in an Ionic Liquid Electrolyte with a Protonated Anion for Lithium Batteries
journal contribution
posted on 2021-06-30, 17:05 authored by Derick Gyabeng, Lixin Qiao, Heng Zhang, Uxue Oteo, Michel Armand, Maria Forsyth, Fangfang Chen, Luke A. O’DellThe
ion associations in two ionic liquid (IL) electrolytes based
on the novel asymmetric anion (difluoromethanesulfonyl) (trifluoromethanesulfonyl)imide
(DFTFSI) are probed in detail using a combination of nuclear magnetic
resonance (NMR) methods [heteronuclear overhauser enhancement spectroscopy
(HOESY), relaxation, and diffusion] and molecular dynamics (MD) simulations.
The 1H–7Li HOESY NMR technique and MD
simulations give insights into the lithium interactions with the IL
anions and cations, while the measured 1H–19F HOESY cross-relaxation rates and MD simulations indicate that the
Li–H (anion) proximity disrupts the hydrogen bonding interaction
previously observed between the DFTFSI anion and the ether oxygen
of the N-methyl-N-methoxyethylpyrrolidinium
(C2O1mpy) cation in the pure IL. Preliminary electrochemical
behavior shows excellent Li compatibility of the C3mpyr
DFTFSI-based IL electrolyte for future lithium-battery applications.