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Advanced Block Copolymer Design for Polymer Electrolytes: Prospects of Microphase Separation

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    Advanced Block Copolymer Design for Polymer Electrolytes: Prospects of Microphase Separation
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    • Andreas J. Butzelaar
      Andreas J. Butzelaar
      Karlsruhe Institute of Technology (KIT), Institute for Chemical Technology and Polymer Chemistry (ITCP), Engesserstraße 18, 76131 Karlsruhe, Germany
      More by Andreas J. Butzelaar
      Orcidhttps://orcid.org/0000-0002-0843-2719
    • Philipp Röring
      Philipp Röring
      Helmholtz-Institute Münster, IEK-12, Forschungszentrum Jülich GmbH, Corrensstraße 46, 48149 Münster, Germany
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    • Maxi Hoffmann
      Maxi Hoffmann
      Karlsruhe Institute of Technology (KIT), Institute for Chemical Technology and Polymer Chemistry (ITCP), Engesserstraße 18, 76131 Karlsruhe, Germany
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    • Jaschar Atik
      Jaschar Atik
      Helmholtz-Institute Münster, IEK-12, Forschungszentrum Jülich GmbH, Corrensstraße 46, 48149 Münster, Germany
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      Orcidhttps://orcid.org/0000-0003-1449-0680
    • Elie Paillard
      Elie Paillard
      Helmholtz-Institute Münster, IEK-12, Forschungszentrum Jülich GmbH, Corrensstraße 46, 48149 Münster, Germany
      Politecnico di Milano, Department of Energy, Via Lambruschini 4, Milan 20156, Italy
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      Orcidhttps://orcid.org/0000-0002-5630-0569
    • Manfred Wilhelm
      Manfred Wilhelm
      Karlsruhe Institute of Technology (KIT), Institute for Chemical Technology and Polymer Chemistry (ITCP), Engesserstraße 18, 76131 Karlsruhe, Germany
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      Orcidhttps://orcid.org/0000-0003-2105-6946
    • Martin Winter
      Martin Winter
      Helmholtz-Institute Münster, IEK-12, Forschungszentrum Jülich GmbH, Corrensstraße 46, 48149 Münster, Germany
      MEET Battery Research Center/Institute of Physical Chemistry, University of Münster, Corrensstraße 46, 48149 Münster, Germany
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    • Gunther Brunklaus
      Gunther Brunklaus
      Helmholtz-Institute Münster, IEK-12, Forschungszentrum Jülich GmbH, Corrensstraße 46, 48149 Münster, Germany
      MEET Battery Research Center/Institute of Physical Chemistry, University of Münster, Corrensstraße 46, 48149 Münster, Germany
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      Orcidhttps://orcid.org/0000-0003-0030-1383
    • Patrick Theato*
      Patrick Theato
      Karlsruhe Institute of Technology (KIT), Institute for Chemical Technology and Polymer Chemistry (ITCP), Engesserstraße 18, 76131 Karlsruhe, Germany
      Karlsruhe Institute of Technology (KIT), Soft Matter Synthesis Laboratory - Institute for Biological Interfaces III (IBG-3), Hermann-von-Helmholtz-Platz 1, 76344 Eggenstein-Leopoldshafen, Germany
      *Email: [email protected]
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      Orcidhttps://orcid.org/0000-0002-4562-9254
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    Macromolecules

    Cite this: Macromolecules 2021, 54, 23, 11101–11112
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    https://doi.org/10.1021/acs.macromol.1c02147
    Published November 26, 2021
    Copyright © 2021 The Authors. Published by American Chemical Society
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    Abstract

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    Herein, we report on an advanced design for polymer electrolytes (PEs) based on our previously reported microphase-separated poly(vinyl benzyl methoxy poly(ethylene oxide) ether)-block-polystyrene block copolymers (PVBmPEO-b-PS). Usually, such block copolymers are characterized by a high mechanical stability provided by the PS domain, while the PEO-based domain features decent ionic conductivities, however, mostly only at higher temperatures. To enable suitable ionic conductivities at lower temperatures, we selectively implemented two ionic liquids (ILs) as a model plasticizer for the PEO domain. Since those ILs are nonmiscible with PS, the latter domain is unaffected, thus still providing a great mechanical stability. To maintain the necessary self-standing film forming ability, we adjusted the size of the PS domain to match with the conducting PEO-based domain. For this, a series of four block copolymers with different PS:PVBmPEO block ratios were synthesized, thus enabling the study of the influence of different amounts of IL. Further, all derived polymer electrolytes were thoroughly characterized by thermal, rheological, morphological, and electrochemical analyses. We could prove the microphase-separated morphology with long-range order and a good thermal and mechanical stability as well as the selective mixing of the ILs within the conducting domain. Consequently, electrochemical impedance spectroscopy revealed a significant increase in ionic conductivity up to 2 orders of magnitude and a reduced interfacial resistance in comparison to a nonplasticized reference sample. Moreover, exhaustive studies of the lithium-ion transference number showed not only the importance of such detailed analysis for IL-containing PEs but also the true increase of the effective lithium-ion conductivity. Finally, we conducted a full cycling in Li||LiFePO4 (LFP) cells to clearly demonstrate the applicability of our approach.

    Copyright © 2021 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/acs.macromol.1c02147.

    • Structure of the ILs, DSC measurement of BPE491:15, additional SAXS measurements, exemplary tLi+ measurement (PDF)

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    This article is cited by 11 publications.

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    2. Ningaraju Gejjiganahalli Ningappa, Anil Kumar Madikere Raghunatha Reddy, Karim Zaghib. Advanced Polymer Electrolytes in Solid-State Batteries. Batteries 2024, 10 (12) , 454. https://doi.org/10.3390/batteries10120454
    3. Dohyun Kim, Rui Sun, Roger Tocchetto, Carl Willis, Bert Krutzer, Frederick L. Beyer, Yossef A. Elabd. Poly(ionic liquid) ABC triblock and ABCBA pentablock terpolymer electrolytes for lithium metal batteries. RSC Applied Polymers 2024, 2 (6) , 1091-1103. https://doi.org/10.1039/D4LP00204K
    4. Tao Feng, Xiang Li, Gang Li, Xinglin Luo, Xingwang Liu, Kun Zhang, Xiaoxia Jia, Yingge Wang, Wei Sun, Kaiying Wang. A low-cost PAN-b-PEG-b-PAN/TEABF4 gel electrolyte for flexible all-solid-state supercapacitors. Journal of Energy Storage 2024, 102 , 114131. https://doi.org/10.1016/j.est.2024.114131
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    6. Anna D. Khudyshkina, Ulf‐Christian Rauska, Andreas J. Butzelaar, Maxi Hoffmann, Manfred Wilhelm, Patrick Theato, Fabian Jeschull. Impact of Nano‐sized Inorganic Fillers on PEO‐based Electrolytes for Potassium Batteries. Batteries & Supercaps 2024, 7 (1) https://doi.org/10.1002/batt.202300404
    7. Jiahao Jiang, Hanyang Gao, Mengjie Wang, Liang Gao, Guoxin Hu. Effect of fillers on the microphase separation in polyurethane composites: A review. Polymer Engineering & Science 2023, 63 (12) , 3938-3962. https://doi.org/10.1002/pen.26507
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    9. Daniel T. Krause, Susanna Krämer, Vassilios Siozios, Andreas J. Butzelaar, Martin Dulle, Beate Förster, Patrick Theato, Joachim Mayer, Martin Winter, Stephan Förster, Hans-Dieter Wiemhöfer, Mariano Grünebaum. Improved Route to Linear Triblock Copolymers by Coupling with Glycidyl Ether-Activated Poly(ethylene oxide) Chains. Polymers 2023, 15 (9) , 2128. https://doi.org/10.3390/polym15092128
    10. Ze-Kun Zhang, Shi-Peng Ding, Ze Ye, Ding-Li Xia, Jun-Ting Xu. PEO-Based Block Copolymer Electrolytes Containing Double Conductive Phases with Improved Mechanical and Electrochemical Properties. Materials 2022, 15 (22) , 7930. https://doi.org/10.3390/ma15227930
    11. André Gröschel, Johannes C. Brendel. Trendbericht Makromolekulare Chemie 2022. Nachrichten aus der Chemie 2022, 70 (10) , 52-63. https://doi.org/10.1002/nadc.20224129512
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    Macromolecules

    Cite this: Macromolecules 2021, 54, 23, 11101–11112
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.macromol.1c02147
    Published November 26, 2021
    Copyright © 2021 The Authors. Published by American Chemical Society
    Request reuse permissions

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