Ion transport in super-concentrated aqueous electrolytes for lithium-ion batteries

Minhaeng Cho, Jonggu Jeon

Research output: Contribution to journalArticlepeer-review

6 Citations (Scopus)


Water-in-salt electrolytes (WiSEs) are a safer alternative to conventional organic electrolytes in battery applications because of their nonflammable nature. The electrochemical performance of these concentrated aqueous solutions of Li electrolytes critically depends on their high electrical conductivity at saturation. Still, the underlying molecular mechanism of Li-ion transport has not yet been clearly elucidated. To better understand this, we investigate four types of predominant atomic interactions and dynamics involving Li ions, anionic oxygen atoms (OT), and atoms of water molecules (OW) in the WiSE made of lithium bis(trifluoromethanesulfonyl)imide with molecular dynamics simulation and theoretical analysis. We present the distribution of atomic composition in the first solvation shells of these atoms and water molecules, thermodynamic stabilities of the contact atom pairs, their lifetimes based on the reactive flux time correlation function and the transition state theory analyses, and the correlation of the Li-ion mobility with the local solvation environment and its dynamics. We find that Li ions follow heterogeneous trajectories on the sub-nanosecond time scale consisting of distinctive water-rich and anion-rich segments, switching between a vehicle-type and a hopping-type mechanism in respective regions. The Li···OW contact pair is slightly more stable than Li···OT at saturation, and this subtle balance appears responsible for the fast Li-ion transport in this class of WiSE.

Original languageEnglish
Pages (from-to)23622-23633
Number of pages12
JournalJournal of Physical Chemistry C
Issue number43
Publication statusPublished - 2021 Nov 4

Bibliographical note

Funding Information:
This work was supported by IBS-R023-D1. We thank J. Kim and Prof. K. Kwak for helpful discussions.

Publisher Copyright:
© 2021 American Chemical Society

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films


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