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Ionic Conductivity Enhancement of Polymer Electrolytes by Directed Crystallization

Cite this: ACS Macro Lett. 2022, 11, 4, 595–602
Publication Date (Web):April 11, 2022
https://doi.org/10.1021/acsmacrolett.2c00040
Copyright © 2022 American Chemical Society

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    Abstract

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    We report that hot stretching of poly(ethylene oxide) (PEO)-based solid polymer electrolytes (SPEs) can lead to a preferred orientation of PEO crystalline lamellae, thereby reducing the tortuosity of the ion-conduction pathway along the thickness direction of the SPE film, causing improved ionic conductivity. The hot stretching method is implemented by stretching SPE films above the melting point of PEO in an inert environment followed by crystallization at room temperature while maintaining the applied strain. The effect of hot stretching on the crystalline orientation, crystallinity, morphology, and ion transport in PEO with two types of salts, lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) and lithium triflate (LiCF3SO3), is investigated in detail. Wide-angle X-ray scattering (WAXS) and small-angle X-ray scattering (SAXS) show that the orientation of PEO crystalline lamellae induces the formation of a short ion-conduction pathway along the through-plane direction of the SPE films, leading to 1.4- to 3.5-fold enhancement in the through-plane ionic conductivity.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsmacrolett.2c00040.

    • Experimental section describing sample preparation methods and characterization techniques; ionic conductivity measurement setup; stress–strain curves; SEM micrographs; neat PEO DSC curve; crystallinity change as a function of strain; azimuthal profiles of PEO crystalline phase and complex crystalline phase; spherical harmonic expansion analysis of 2D SAXS pattern (PDF)

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    Cited By

    This article is cited by 3 publications.

    1. Lu Lin, Zening Liu, Uvinduni I. Premadasa, Tianyu Li, Ying-Zhong Ma, Robert L. Sacci, John Katsaras, Kunlun Hong, C. Patrick Collier, Jan-Michael Y. Carrillo, Benjamin Doughty. The Unexpected Role of Cations in the Self-Assembly of Positively Charged Amphiphiles at Liquid/Liquid Interfaces. The Journal of Physical Chemistry Letters 2022, 13 (46) , 10889-10896. https://doi.org/10.1021/acs.jpclett.2c02921
    2. Sun Theo Constan Lotebulo Ndruru, Sonny Widiarto, Edi Pramono, Deana Wahyuningrum, Bunbun Bundjali, I Made Arcana. Modification of Nias’ Cacao Pod Husk Cellulose through Carboxymethylation Stages by Using MAOS Method and Its Application as Li‐ion Batteries’ Biopolymer Electrolyte Membrane**. ChemistrySelect 2022, 7 (44) https://doi.org/10.1002/slct.202202510
    3. Qiancheng Zhu, Chun Ye, Deyu Mao. Solid-State Electrolytes for Lithium–Sulfur Batteries: Challenges, Progress, and Strategies. Nanomaterials 2022, 12 (20) , 3612. https://doi.org/10.3390/nano12203612

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