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Rationally Designed PEGDA–LLZTO Composite Electrolyte for Solid-State Lithium Batteries

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    Energy, Environmental, and Catalysis Applications

    Rationally Designed PEGDA–LLZTO Composite Electrolyte for Solid-State Lithium Batteries
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    • Xingwen Yu
      Xingwen Yu
      Materials Science and Engineering Program and Texas Materials Institute, The University of Texas at Austin, Austin, Texas 78712, United States
      More by Xingwen Yu
    • Yijie Liu
      Yijie Liu
      Materials Science and Engineering Program and Texas Materials Institute, The University of Texas at Austin, Austin, Texas 78712, United States
      More by Yijie Liu
    • John B. Goodenough
      John B. Goodenough
      Materials Science and Engineering Program and Texas Materials Institute, The University of Texas at Austin, Austin, Texas 78712, United States
      More by John B. Goodenough
      Orcidhttps://orcid.org/0000-0001-9350-3034
    • Arumugam Manthiram*
      Arumugam Manthiram
      Materials Science and Engineering Program and Texas Materials Institute, The University of Texas at Austin, Austin, Texas 78712, United States
      *Email: [email protected]
      More by Arumugam Manthiram
      Orcidhttps://orcid.org/0000-0003-0237-9563
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2021, 13, 26, 30703–30711
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    https://doi.org/10.1021/acsami.1c07547
    Published June 28, 2021
    Copyright © 2021 American Chemical Society
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    Abstract

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    A novel composite electrolyte is rationally designed with a polyethylene glycol diacrylate (PEGDA) polymer and a garnet-type fast lithium-ion conductor (Li6.4La3Zr1.4Ta0.6O12, LLZTO) for solid-state lithium batteries. The LLZTO ceramic phase is incorporated into the PEGDA polymeric matrix as nanoparticles. The ionic conductivity of the composite is further optimized with a succinonitrile plasticizer. The solid composite membranes are synthesized via a tape casting process followed by a UV curing procedure. The resulting solid-state composite electrolyte delivers a room-temperature Li+-ion conductivity of 3.1 × 10–4 S cm–1 and can sustain an electrochemical polarization potential up to 4.6–4.7 V (vs Li+/Li). The compositing approach harnesses the advantages of both polymeric PEGDA and ceramic LLZTO. In addition to enhancing the ionic conductivity, the LLZTO ceramic filler can suppress Li dendrites. The polymeric phase of PEGDA facilitates good interfacial contact between the solid electrolyte and the electrodes. The solid-state cells fabricated with the composite solid electrolyte, lithium–metal anode, and LiNi0.8Mn0.1Co0.1O2 (NMC 811) cathode show long cyclability.

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    • Schematic of synthesizing the PEGDA–SCN–LiTFSI polymeric electrolytes; schematic of a Swagelok symmetric cell with two stainless-steel rods and an equivalent circuit for the electrochemical impedance spectrum of the electrolyte membranes; picture of a PEGDA–SCN–LiTFSI polymeric membrane; SEM images of the synthesized LLZTO powder after the first-step sintering and after the second-step sintering; schematic of synthesizing the PEGDA–SCN–LiTFSI–LLZTO composite electrolytes; picture of a piece of the PEGDA–SCN–LiTFSI–LLZTO composite membrane; ATR–FTIR profile of a PEGDA–SCN membrane; SEM image of the NMC 811 cathode powder; and XRD characteristics of the NMC 811 cathode (PDF)

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    Cite this: ACS Appl. Mater. Interfaces 2021, 13, 26, 30703–30711
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    https://doi.org/10.1021/acsami.1c07547
    Published June 28, 2021
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