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Peer-reviewedCC BY 4.0JPhys Energy

Structural dynamics drive mobility in water-in-salt electrolytes

Abstract

Water-in-salt electrolytes (WISE) defy classical transport models by maintaining high ionic conductivity despite extreme viscosities. Here, we uncover the multiscale mechanisms behind this anomaly in superconcentrated aqueous Lithium bis(trifluoromethane)sulfonimide (LiTFSI) solutions. Using viscosity and conductivity measurements alongside pulsed-field gradient nuclear magnetic resonance and Quasi Elastic Neutron Scattering (QENS), we reveal a pronounced decoupling between species mobility and bulk viscosity. Lithium species and protons retain high mobility, while TFSI − anions are increasingly hindered. QENS identifies transient, water-rich nanodomains that enable rapid local diffusion and dynamic interdomain exchange. This work provides direct experimental evidence for hierarchical, decoupled transport in WISE, offering a new framework for designing high-performance electrolytes for energy storage.

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BibTeX
@article{doublet2026structural,
  title = {{Structural dynamics drive mobility in water-in-salt electrolytes}},
  author = {Célia Doublet and Claire Villevieille and Lauréline Lecarme and Patrick Judeinstein and Agathe Bélime and Jan Peter Embs and Markus Appel and Sandrine Lyonnard and Fannie Alloin and Quentin Berrod},
  journal = {JPhys Energy},
  year = {2026},
  month = oct,
  doi = {10.1088/2515-7655/aea9c8},
  url = {https://hal.science/hal-05801397v1},
  note = {CC BY 4.0},
}
RIS
TY  - JOUR
TI  - Structural dynamics drive mobility in water-in-salt electrolytes
AU  - Célia Doublet
AU  - Claire Villevieille
AU  - Lauréline Lecarme
AU  - Patrick Judeinstein
AU  - Agathe Bélime
AU  - Jan Peter Embs
AU  - Markus Appel
AU  - Sandrine Lyonnard
AU  - Fannie Alloin
AU  - Quentin Berrod
PY  - 2026
DA  - 2026/10/08
JO  - JPhys Energy
DO  - 10.1088/2515-7655/aea9c8
UR  - https://hal.science/hal-05801397v1
AB  - Water-in-salt electrolytes (WISE) defy classical transport models by maintaining high ionic conductivity despite extreme viscosities. Here, we uncover the multiscale mechanisms behind this anomaly in superconcentrated aqueous Lithium bis(trifluoromethane)sulfonimide (LiTFSI) solutions. Using viscosity and conductivity measurements alongside pulsed-field gradient nuclear magnetic resonance and Quasi Elastic Neutron Scattering (QENS), we reveal a pronounced decoupling between species mobility and bulk viscosity. Lithium species and protons retain high mobility, while TFSI − anions are increasingly hindered. QENS identifies transient, water-rich nanodomains that enable rapid local diffusion and dynamic interdomain exchange. This work provides direct experimental evidence for hierarchical, decoupled transport in WISE, offering a new framework for designing high-performance electrolytes for energy storage.
SN  - 2515-7655
ER  -