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A Polysiloxane-Enabled Ternary Eutectic Electrolyte with Fast Ion Transport under Extreme Conditions

  • Weiping Li
    Weiping Li
    School of Chemical Science and Technology, Yunnan University, Kunming 650091, China
    Division of Natural and Applied Sciences, Duke Kunshan University, Kunshan, Jiangsu 215306, China
    More by Weiping Li
  • Peng Wen
    Peng Wen
    School of Chemical Science and Technology, Yunnan University, Kunming 650091, China
    State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Fudan University, Shanghai 200433, China
    More by Peng Wen
  • Yang Ren
    Yang Ren
    School of Chemical Science and Technology, Yunnan University, Kunming 650091, China
    More by Yang Ren
  • Wen Xie
    Wen Xie
    School of Chemical Science and Technology, Yunnan University, Kunming 650091, China
    More by Wen Xie
  • Jun Lin
    Jun Lin
    School of Chemical Science and Technology, Yunnan University, Kunming 650091, China
    More by Jun Lin
  • Mao Chen
    Mao Chen
    State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Fudan University, Shanghai 200433, China
    More by Mao Chen
  • Yuan Yang*
    Yuan Yang
    Department of Applied Physics and Applied Mathematics, Columbia University, New York, New York 10027, United States
    *[email protected]
    More by Yuan Yang
  • , and 
  • Xinrong Lin*
    Xinrong Lin
    School of Chemical Science and Technology, Yunnan University, Kunming 650091, China
    Division of Natural and Applied Sciences, Duke Kunshan University, Kunshan, Jiangsu 215306, China
    *[email protected]
    More by Xinrong Lin
Cite this: ACS Energy Lett. 2023, 8, 12, 5128–5135
Publication Date (Web):November 16, 2023
https://doi.org/10.1021/acsenergylett.3c01558
Copyright © 2023 American Chemical Society

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    Abstract

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    Developing lithium–metal batteries under extreme conditions is highly challenging and requires flammable/volatile solvents. In pursuit of safe electrolyte materials, polymers possess slow lithium transport, while eutectic electrolytes (EEs) suffer from interfacial instability, impeding their applications under extreme conditions. Herein, we report that addition of a designed brush-polysiloxane into EE unexpectedly boosted ionic conductivity by nearly 3-fold to 0.59 mS cm–1 at −40 °C compared to that without polymer, fulfilling fast transport kinetics. Spectroscopic characterizations and simulations revealed formation of a ternary EE via intermolecular interactions as well as a stabilized interface, which successfully led to a high capacity of 149 mAh g–1 at −40 °C (85% of room-temperature capacity) and stable fast-charging performance up to 1,000 mA g–1 (6 min recharging) over 100 cycles in Li||LiNi0.6Co0.2Mn0.2O2 cells. The polymer-enhanced electrolyte offers a paradigm shift approach to tune kinetics in high-performance and safe lithium batteries under extreme conditions.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsenergylett.3c01558.

    • Synthetic method, 1H NMR spectra, optical images of eutectic electrolytes, CV curves, EIS data, rheological data, SEM images, Raman spectra, FT-IR spectra, XPS spectra, DFT calculation method (PDF)

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