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Comb Polymers with Triazole Linkages under Thermal and Mechanical Stress

  • Charlotte Petit
    Charlotte Petit
    School of Chemistry, Physics and Mechanical Engineering, Queensland University of Technology (QUT), 2 George Street, Brisbane, QLD 4000, Australia
    Macromolecular Architectures, Institut für Technische Chemie and Polymerchemie, Karlsruhe Institute of Technology (KIT), Engesserstr. 18, 76128 Karlsruhe, Germany
  • Mahdi Abbasi
    Mahdi Abbasi
    Polymeric Materials, Institut für Technische Chemie und Polymerchemie, Karlsruhe Institute of Technology (KIT), Engesserstr. 18, 76128 Karlsruhe, Germany
    More by Mahdi Abbasi
  • Tobias S. Fischer
    Tobias S. Fischer
    School of Chemistry, Physics and Mechanical Engineering, Queensland University of Technology (QUT), 2 George Street, Brisbane, QLD 4000, Australia
    Macromolecular Architectures, Institut für Technische Chemie and Polymerchemie, Karlsruhe Institute of Technology (KIT), Engesserstr. 18, 76128 Karlsruhe, Germany
  • Manfred Wilhelm*
    Manfred Wilhelm
    Polymeric Materials, Institut für Technische Chemie und Polymerchemie, Karlsruhe Institute of Technology (KIT), Engesserstr. 18, 76128 Karlsruhe, Germany
    *E-mail: [email protected] (M.W.).
  • Anja S. Goldmann*
    Anja S. Goldmann
    School of Chemistry, Physics and Mechanical Engineering, Queensland University of Technology (QUT), 2 George Street, Brisbane, QLD 4000, Australia
    Macromolecular Architectures, Institut für Technische Chemie and Polymerchemie, Karlsruhe Institute of Technology (KIT), Engesserstr. 18, 76128 Karlsruhe, Germany
    *E-mail: [email protected] (A.S.G.).
  • , and 
  • Christopher Barner-Kowollik*
    Christopher Barner-Kowollik
    School of Chemistry, Physics and Mechanical Engineering, Queensland University of Technology (QUT), 2 George Street, Brisbane, QLD 4000, Australia
    Macromolecular Architectures, Institut für Technische Chemie and Polymerchemie, Karlsruhe Institute of Technology (KIT), Engesserstr. 18, 76128 Karlsruhe, Germany
    *E-mail: [email protected] (C.B.-K.).
Cite this: Macromolecules 2019, 52, 2, 420–431
Publication Date (Web):January 3, 2019
https://doi.org/10.1021/acs.macromol.8b02174
Copyright © 2019 American Chemical Society

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    Abstract

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    Assessing the stability of molecular bonds in polymer architectures is of critical importance for determining conditions for extrusion, molding, and processing. The topological complexity of branched polymers defines their strain hardening and consequently their melt strength properties, critical parameters for their exploitation in applications. Their molecular architecture is defined by the grafting density and the chain length of the backbone as well as branches. Herein, we introduce a set of polymer combs to establish an understanding of the above parameters on the stability of the popular triazole linkage—often exploited in tethering the branches to the backbone—during thermal treatment and shearing. We exploit a combination of reversible deactivation radical polymerization (RDRP) and copper-catalyzed alkyne–azide cycloaddition (CuAAC) to construct comb polymers (ranging in backbone number-average molecular weight from 39.9 to 55.6 kg mol–1 and a branch length from 3.3 to 18 kg mol–1) with statistically located branches tethered via triazole-based ligation to the backbone. These polymer combs were subsequently thermally challenged at 150 °C (or 180 °C) in an inert atmosphere as well as subjected to shearing at the same temperature. The resulting molecular cleavage processes were analyzed via size exclusion chromatography (SEC) as well as SEC coupled to high-resolution electrospray ionization mass spectrometry (SEC-HR ESI MS) to establish a mechanistic image of branch debonding when it occurs. In addition, by virtue of this approach, we establish an in-depth understanding of how the comb architecture dictates its stability under otherwise unchanged chemical bonding conditions via triazole units, allowing to adopt design criteria for generating thermally and mechanically stable comb structures.

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    The Supporting Information is available free of charge on the ACS Publications Web site at DOI: 10.1021/acs.macromol.xxx. (PDF). The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.macromol.8b02174.

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    Cited By

    This article is cited by 2 publications.

    1. Mingqiu Hu, Xindi Li, Javid Rzayev, Thomas P. Russell. Hydrolysis-Induced Self-Assembly of High-χ–Low-N Bottlebrush Copolymers. Macromolecules 2021, 54 (24) , 11449-11458. https://doi.org/10.1021/acs.macromol.1c02061
    2. Steve Neumann, Michel Biewend, Sravendra Rana, Wolfgang H. Binder. The CuAAC: Principles, Homogeneous and Heterogeneous Catalysts, and Novel Developments and Applications. Macromolecular Rapid Communications 2020, 41 (1) https://doi.org/10.1002/marc.201900359

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