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Improving the Strength of Ultrastiff Organic–Inorganic Double-Network Hydrogels

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    Improving the Strength of Ultrastiff Organic–Inorganic Double-Network Hydrogels
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    • Marko Milovanovic
      Marko Milovanovic
      Biomaterials and Polymer Science, Department of Bio- and Chemical Engineering, TU Dortmund, Emil-Figge-Str. 66, 44227 Dortmund, Germany
      More by Marko Milovanovic
    • Nicola Isselbaecher
      Nicola Isselbaecher
      Biomaterials and Polymer Science, Department of Bio- and Chemical Engineering, TU Dortmund, Emil-Figge-Str. 66, 44227 Dortmund, Germany
      More by Nicola Isselbaecher
    • Volker Brandt
      Volker Brandt
      Biomaterials and Polymer Science, Department of Bio- and Chemical Engineering, TU Dortmund, Emil-Figge-Str. 66, 44227 Dortmund, Germany
      More by Volker Brandt
    • Joerg C. Tiller*
      Joerg C. Tiller
      Biomaterials and Polymer Science, Department of Bio- and Chemical Engineering, TU Dortmund, Emil-Figge-Str. 66, 44227 Dortmund, Germany
      *Email: [email protected]
      More by Joerg C. Tiller
      Orcidhttps://orcid.org/0000-0002-1531-0795
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    Chemistry of Materials

    Cite this: Chem. Mater. 2021, 33, 21, 8312–8322
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    https://doi.org/10.1021/acs.chemmater.1c02525
    Published October 19, 2021
    Copyright © 2021 The Authors. Published by American Chemical Society
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    Abstract

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    Swollen double networks (DNs) are hydrogels with greatly improved stiffness, toughness, and strength compared to classical hydrogels. The highest stiffness is achieved for organic–inorganic DN hydrogels, which show a rather low tensile strength of about 1 MPa so far. It was presumed that this is due to an insufficient reversible bond formation between inorganic and organic phases. Therefore, the influence of the functional groups that form reversible bonds between these two phases was investigated on the example of calcium phosphate-based DN hydrogels. The functional groups were introduced by copolymerization of acrylate-based monomers with acrylamide and N,N- dimethylacrylamide, respectively, to form a hydrogel-containing alkaline phosphatase. After enzyme-induced mineralization, it was found that only acrylic acid (AA) results in improved strength of the formed ultrastiff DN hydrogels. Stress–strain curves with different strain rates revealed that Young’s modulus of ∼300 MPa is constant in all cases, while the tensile strength increases from 7 MPa at 5% min–1 to 17 MPa at 750% min–1. The fracture toughness of these optically transparent DN hydrogels, which are among the stiffest and strongest existing hydrogels, is up to 2000 J m–2 which is also improved by the introduction of AA into the hydrogel.

    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.chemmater.1c02525.

    • Network compositions, mineralization parameters, and mechanical properties of the mineralized DNHs; EDX measurement; Compression curve of one exemplary mineralized DNH (PDF)

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    Chemistry of Materials

    Cite this: Chem. Mater. 2021, 33, 21, 8312–8322
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.chemmater.1c02525
    Published October 19, 2021
    Copyright © 2021 The Authors. Published by American Chemical Society
    Request reuse permissions

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