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Non-Newtonian Dynamics in Water-in-Salt Electrolytes
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    Non-Newtonian Dynamics in Water-in-Salt Electrolytes
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    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2024, 15, 1, 76–80
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    https://doi.org/10.1021/acs.jpclett.3c03145
    Published December 22, 2023
    Copyright © 2023 American Chemical Society

    Abstract

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    Water-in-salt electrolytes have attracted considerable interest in the past decade for advanced lithium-ion batteries, possessing important advantages over the non-aqueous electrolytes currently in use. A battery with a LiTFSI–water electrolyte was demonstrated in which an operating window of 3 V is made possible by a solid–electrolyte interface. Viscosity is an important property for such electrolytes, because high viscosity is normally associated with low ionic conductivity. Here, we investigate shear and longitudinal viscosities using shear stress and compressional longitudinal stress measurements as functions of frequency and concentration. We find that both viscosities are frequency-dependent and exhibit almost identical frequency and concentration dependences in the high-concentration region. A comparison to quasielastic neutron scattering experiments suggests that both are governed by structural relaxation of the TFSI network. Thus, LiFTSI–water electrolytes appear to be an unusual case of a non-Newtonian fluid, where shear and longitudinal viscosities are determined by the same relaxation mechanism.

    Copyright © 2023 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpclett.3c03145.

    • Neutron-weighted average interference functions for 21 m LiTFSI–H2O (Figure S1); calculation of the function G(Q, υ) displayed in Figure 4 of the main paper (PDF)

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    This article is cited by 3 publications.

    1. Tsuyoshi Yamaguchi. Molecular Dynamics Simulation Study on Heterogeneous Structure, Rheology, and Dynamic Correlation of Concentrated Aqueous Solutions of a Lithium Salt. The Journal of Physical Chemistry B 2025, 129 (3) , 1026-1035. https://doi.org/10.1021/acs.jpcb.4c07942
    2. Antonio Faraone, Fei Wang, Saya Takeuchi, Joseph A. Dura. Structural Relaxation and Nanodomain Dynamics in Highly Concentrated Electrolytes for Zinc Batteries. The Journal of Physical Chemistry C 2024, 128 (29) , 12121-12130. https://doi.org/10.1021/acs.jpcc.4c00360
    3. Yiwei Jiang, Theo G. M. van de Ven. Cations and Anions Affect the Speed of Sound in Water Oppositely. The Journal of Physical Chemistry Letters 2024, 15 (15) , 4125-4129. https://doi.org/10.1021/acs.jpclett.4c00318

    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2024, 15, 1, 76–80
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpclett.3c03145
    Published December 22, 2023
    Copyright © 2023 American Chemical Society

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