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Polynorbornene-Based Polyelectrolytes with Covalently Attached Metallacarboranes: Synthesis, Characterization, and Lithium-Ion Mobility

Cite this: Macromolecules 2021, 54, 14, 6867–6877
Publication Date (Web):June 17, 2021
https://doi.org/10.1021/acs.macromol.1c00350
Copyright © 2021 American Chemical Society

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    Abstract

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    Metallacarborane clusters, such as COSAN, belong to surface-active and low-coordinating nanosized anions. Therefore, they have been used as separate building blocks in self- and co-assembly. As a step forward, we synthesized via ring-opening metathesis polymerization a novel polyelectrolyte, poly(norbornene-COSAN), PNC, with metallacarborane anions covalently attached to a polynorbornene backbone. The resulting PNC, with the degree of polymerization around 120, is soluble in polar organic solvents, and it can be deposited on a substrate as separate polymer chains or as multichain aggregates, with the bundle-of-fibril patterning. PNC is miscible with polyethylene oxide (PEO), forming the PNC/PEO composite. As shown by solid-state nuclear magnetic resonance spectroscopy, Li+ counterions are firmly coordinated in the PNC matrix, exhibiting rather restricted dynamics. In contrast, the mixing of PNC with PEO leads to a substantial increase of Li+ dynamics. As the result, the mobility of Li+ in the PNC/PEO composite remains almost unrestrained, which makes the COSAN-containing polyelectrolytes promising candidates for ion-conducting materials.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.macromol.1c00350.

    • Structure of Monomer, PNC, and PNC/PEO samples and their characterization by NMR, ESI MS, TGA, DSC, and XRD and additional data and images from AFM, TEM, STEM, and ss-NMR analyses (PDF)

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    Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

    This article is cited by 4 publications.

    1. Žiga Medoš, Belhssen Hleli, Zdeněk Tošner, Peter Ogrin, Tomaž Urbič, Ksenija Kogej, Marija Bešter-Rogač, Pavel Matějíček. Counterion-Induced Aggregation of Metallacarboranes. The Journal of Physical Chemistry C 2022, 126 (12) , 5735-5742. https://doi.org/10.1021/acs.jpcc.2c00107
    2. Mustafa Ahmed, Dung T. Tran, John Putziger, Zhifan Ke, Ashkan Abtahi, Zhiyang Wang, Ke Chen, Kai Lang, Jianguo Mei. Tetracyanocyclopentadienide-Based Stable Poly(aromatic) Anions. ACS Macro Letters 2022, 11 (1) , 72-77. https://doi.org/10.1021/acsmacrolett.1c00711
    3. Zhuo-Qun Lu, Lan-Lan Zhang, Yukun Yan, Wei Wang. Polyelectrolytes of Inorganic Polyoxometalates: Acids, Salts, and Complexes. Macromolecules 2021, 54 (14) , 6891-6900. https://doi.org/10.1021/acs.macromol.1c00783
    4. James McQuade, Mya I. Serrano, Frieder Jäkle. Main group functionalized polymers through ring-opening metathesis polymerization (ROMP). Polymer 2022, 246 , 124739. https://doi.org/10.1016/j.polymer.2022.124739