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Toward High-Capacity Li–S Solid-State Batteries: The Role of Partial Ionic Transport in the Catholyte
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    Toward High-Capacity Li–S Solid-State Batteries: The Role of Partial Ionic Transport in the Catholyte
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    • Henry M. Woolley
      Henry M. Woolley
      MEET Battery Research Center, Institute of Physical Chemistry, University of Münster, Corrensstraße 46, 48149, Münster, Germany
      International Graduate School for Battery Chemistry, Characterization, Analysis, Recycling and Application (BACCARA), University of Münster, Corrensstraße 40, 48149 Münster, Germany
    • Martin Lange
      Martin Lange
      Insitute of Inorganic and Analytical Chemistry, University of Münster, Corrensstraße 28/30, 48149 Münster, Germany
      More by Martin Lange
    • Elina Nazmutdinova
      Elina Nazmutdinova
      International Graduate School for Battery Chemistry, Characterization, Analysis, Recycling and Application (BACCARA), University of Münster, Corrensstraße 40, 48149 Münster, Germany
      Insitute of Inorganic and Analytical Chemistry, University of Münster, Corrensstraße 28/30, 48149 Münster, Germany
    • Nella M. Vargas-Barbosa*
      Nella M. Vargas-Barbosa
      Chair of Electrochemistry, University of Bayreuth and Bavarian Center for Battery Technology (BayBatt), Universitätsstrasse 30, 95447 Bayreuth, Germany
      *Email: [email protected]
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    ACS Energy Letters

    Cite this: ACS Energy Lett. 2024, 9, 7, 3547–3556
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    https://doi.org/10.1021/acsenergylett.4c01444
    Published June 28, 2024
    Copyright © 2024 American Chemical Society

    Abstract

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    To address the challenges of tortuous partial ionic transport and chemomechanical failure due to the large volumetric changes of sulfur during all-solid-state battery cycling, we evaluate a hybrid electrolyte composed of the lithium chloride argyrodite Li6PS5Cl (LPSCl) and an ionic liquid-based lithium liquid electrolyte (ILE) in the cathode composite of Li–S half-cells. We confirm the stability of the LPSCl/ILE interface by coupling Raman and impedance spectroscopy measurements. Charge–discharge curves show a capacity improvement for the hybrid cells (1364 ± 151 mAh·g–1), compared to 904 ± 186 mAh·g–1 for pristine cells. Transport measurements quantify an increase in the partial ionic conductivity of proxy cathode layers from 0.2 to 0.4 mS·cm–1 in hybrid cells. Taken together, the use of the ILE increases the partial ionic transport and access to sulfur which results in higher and more stable discharge capacities.

    Copyright © 2024 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/acsenergylett.4c01444.

    • Detailed experimental methods, additional impedance spectra and impedance fitting results, further Raman spectra, scanning electron microscopy images and corresponding energy dispersive X-ray elemental analyses, differential capacity plots, and DC polarization results (PDF)

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    This article is cited by 2 publications.

    1. Tao Yu, Yuankai Liu, Haoyu Li, Yu Sun, Shaohua Guo, Haoshen Zhou. Ductile Inorganic Solid Electrolytes for All-Solid-State Lithium Batteries. Chemical Reviews 2025, Article ASAP.
    2. Saneyuki OHNO. Toward the Use of Composite Cathode with Significantly High Interfacial Area Density for Solid-State Li–S Batteries. Denki Kagaku 2024, 92 (4) , 330-335. https://doi.org/10.5796/denkikagaku.24-FE0407

    ACS Energy Letters

    Cite this: ACS Energy Lett. 2024, 9, 7, 3547–3556
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsenergylett.4c01444
    Published June 28, 2024
    Copyright © 2024 American Chemical Society

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