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pH-Responsive Saloplastics Based on Weak Polyelectrolytes: From Molecular Processes to Material Scale Properties

  • Gaulthier Rydzek*
    Gaulthier Rydzek
    World Premier International Center for Materials Nanoarchitectonics (MANA), National Institute for Materials Science (NIMS), Tsukuba, Japan
    Centre for Research on Adaptive Nanostructures and Nanodevices (CRANN) and Advanced Materials Bio-Engineering Research Centre (AMBER), School of Chemistry, Trinity College Dublin, Dublin, Ireland
    *E-mail [email protected] (G.R.).
  • Amir Pakdel
    Amir Pakdel
    Centre for Research on Adaptive Nanostructures and Nanodevices (CRANN) and Advanced Materials Bio-Engineering Research Centre (AMBER), School of Chemistry, Trinity College Dublin, Dublin, Ireland
    More by Amir Pakdel
  • Agnieszka Witecka
    Agnieszka Witecka
    Institute of Fundamental Technological Research, Polish Academy of Sciences, Warsaw, Poland
  • Dayangku Noorfazidah Awang Shri
    Dayangku Noorfazidah Awang Shri
    Faculty of Mechanical Engineering, Universiti Malaysia Pahang, Pekan, Pahang, Malaysia
  • Fabien Gaudière
    Fabien Gaudière
    CNRS, Institut Charles Sadron UPR 22, Université de Strasbourg, F-67000 Strasbourg, France
  • Valeria Nicolosi
    Valeria Nicolosi
    Centre for Research on Adaptive Nanostructures and Nanodevices (CRANN) and Advanced Materials Bio-Engineering Research Centre (AMBER), School of Chemistry, Trinity College Dublin, Dublin, Ireland
  • Parvaneh Mokarian-Tabari
    Parvaneh Mokarian-Tabari
    Centre for Research on Adaptive Nanostructures and Nanodevices (CRANN) and Advanced Materials Bio-Engineering Research Centre (AMBER), School of Chemistry, Trinity College Dublin, Dublin, Ireland
  • Pierre Schaaf
    Pierre Schaaf
    UMR-S 1121, Biomatériaux et Bioingénierie, Institut National de la Santé et de la Recherche Médicale, 11 rue Humann, Cedex 67085 Strasbourg, France
  • Fouzia Boulmedais
    Fouzia Boulmedais
    CNRS, Institut Charles Sadron UPR 22, Université de Strasbourg, F-67000 Strasbourg, France
  • , and 
  • Katsuhiko Ariga
    Katsuhiko Ariga
    World Premier International Center for Materials Nanoarchitectonics (MANA), National Institute for Materials Science (NIMS), Tsukuba, Japan
    Graduate School of Frontier Sciences, The University of Tokyo, Kashiwa 277-0827, Japan
Cite this: Macromolecules 2018, 51, 12, 4424–4434
Publication Date (Web):June 4, 2018
https://doi.org/10.1021/acs.macromol.8b00609
Copyright © 2018 American Chemical Society

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    Abstract

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    Compact polyelectrolyte complexes (COPECs), also named saloplastics, represent a new class of material with high fracture strain and self-healing properties. Here, COPECs based on poly(methacrylic acid) (PMAA) and poly(allylamine hydrochloride) (PAH) were prepared by centrifugation at pH 7. The influence of postassembly pH changes was monitored chemically by ATR-FTIR, ICP, DSC, and TGA, morphologically by SEM, and mechanically by strain to break measurements. Postassembly pH stimuli misbalanced the charge ratio in COPECs, impacting their concentration in counterions, cross-link density, and polymer chain mobility. At the material level, changes were observed in the porosity, composition, water content, and mechanical properties of COPECs. The cross-link density was a prominent factor governing the saloplastic’s composition and water content. However, the porosity and mechanical properties were driven by several factors including salt-induced plasticization and conformational changes of polyelectrolytes. This work illustrates how multiple-scale consequences arise from a single change in the environment of COPECs, providing insights for future design of stimuli-responsive materials.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.macromol.8b00609.

    • ATR-FTIR spectra of COPECs (raw and deconvoluted spectra), XPS, TGA, DSC, and detailed calculations of bCOOpH (PDF)

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