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Comparative Study of the Mechanical Reinforcement by Blending, Filling, and Block Copolymerization in Bottlebrush Polymer Electrolytes
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    Comparative Study of the Mechanical Reinforcement by Blending, Filling, and Block Copolymerization in Bottlebrush Polymer Electrolytes
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    • Jannik Petry
      Jannik Petry
      Applied Functional Polymers, University of Bayreuth, Universitätsstraße 30, 95447 Bayreuth, Germany
      More by Jannik Petry
    • Harimohan Erabhoina
      Harimohan Erabhoina
      Applied Functional Polymers, University of Bayreuth, Universitätsstraße 30, 95447 Bayreuth, Germany
    • Markus Dietel
      Markus Dietel
      Applied Functional Polymers, University of Bayreuth, Universitätsstraße 30, 95447 Bayreuth, Germany
    • Mukundan Thelakkat*
      Mukundan Thelakkat
      Applied Functional Polymers, University of Bayreuth, Universitätsstraße 30, 95447 Bayreuth, Germany
      Bavarian Polymer Institute (BPI), University of Bayreuth, Universitätsstraße 30, 95447 Bayreuth, Germany
      Bavarian Center for Battery Technology (BayBatt), University of Bayreuth, Universitätsstraße 30, 95447 Bayreuth, Germany
      *Email: [email protected]
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    ACS Applied Polymer Materials

    Cite this: ACS Appl. Polym. Mater. 2024, 6, 9, 5109–5120
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    https://doi.org/10.1021/acsapm.4c00161
    Published April 29, 2024
    Copyright © 2024 The Authors. Published by American Chemical Society

    Abstract

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    Poly(ethylene glycol) (PEG)-based bottlebrush polymer electrolytes exhibit improved room-temperature ionic conductivity and reduced crystallinity compared to those of semicrystalline poly(ethylene oxide) (PEO). However, these graft copolymers suffer from low mechanical stability. Therefore, we synthesized a PEG-based bottlebrush polymer having a polynorbornene backbone using ring-opening metathesis polymerization, and it was mechanically reinforced using three strategies: (a) by blending with a polynorbornene (PNb) homopolymer, (b) filling with TiO2 nanoparticles, or (c) via block copolymerization with a PNb segment. All three systems were converted to solid polymer electrolytes by adding LiTFSI, and their thermal, mechanical, and detailed electrochemical properties in symmetrical Li/SPE/Li cells over a large number of cycles are given. All solid-state lithium metal battery (Li/SPE/LFP) cells were fabricated, and charge/discharge cycles as well as the cycling behavior were comparatively studied. It was found that block copolymerization resulted in the highest storage modulus above 0.1 Hz and overall ionic conductivity (in the whole range of 25 to 80 °C) compared to those of the other two strategies. Furthermore, the highest accessible discharge capacities (159 mA h g–1) and highest capacity retention of 88% after 50 cycles were also achieved with the block copolymer concept.

    Copyright © 2024 The Authors. Published by 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/acsapm.4c00161.

    • Materials, instrumentation, syntheses, 1H NMR spectra, polymer and electrolyte composition, SEC elugrams, thermal analysis, SEM images, rheology measurements, lithium transference number determination, and LPS experiments (PDF)

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    Cited By

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    This article is cited by 2 publications.

    1. Jannik Petry, Markus Dietel, Mukundan Thelakkat. Semi‐Interpenetrating Network Electrolytes Utilizing Ester‐Functionalized Low T g Polysiloxanes in Lithium‐Metal Batteries. Advanced Energy Materials 2024, 13 https://doi.org/10.1002/aenm.202403531
    2. Dong Liu, Shangming He, Longfei Luo, Weilu Yang, Yun Liu, Shichu Yang, Zhihao Shen, Shuangjun Chen, Xing-He Fan. Double gyroid-structured electrolyte based on an azobenzene-containing monomer and its polymer. Soft Matter 2024, 20 (32) , 6424-6430. https://doi.org/10.1039/D4SM00551A

    ACS Applied Polymer Materials

    Cite this: ACS Appl. Polym. Mater. 2024, 6, 9, 5109–5120
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsapm.4c00161
    Published April 29, 2024
    Copyright © 2024 The Authors. Published by American Chemical Society

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