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Tuning the Self-Healing Response of Poly(dimethylsiloxane)-Based Elastomers

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    Tuning the Self-Healing Response of Poly(dimethylsiloxane)-Based Elastomers
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    • Diana Döhler*
      Diana Döhler
      Macromolecular Chemistry, Division of Technical and Macromolecular Chemistry, Institute of Chemistry, Faculty of Natural Sciences II (Chemistry, Physics and Mathematics), Martin Luther University Halle-Wittenberg, von-Danckelmann-Platz 4, Halle D-06120, Germany
      Department of Chemical Engineering, Stanford University, 443 Via Ortega, Stanford, California 94305, United States
      *(D.D.) Email: [email protected]
      More by Diana Döhler
      Orcidhttp://orcid.org/0000-0003-4996-1892
    • Jiheong Kang
      Jiheong Kang
      Department of Chemical Engineering, Stanford University, 443 Via Ortega, Stanford, California 94305, United States
      Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
      More by Jiheong Kang
    • Chris Brittain Cooper
      Chris Brittain Cooper
      Department of Chemical Engineering, Stanford University, 443 Via Ortega, Stanford, California 94305, United States
      More by Chris Brittain Cooper
    • Jeffrey B.-H. Tok
      Jeffrey B.-H. Tok
      Department of Chemical Engineering, Stanford University, 443 Via Ortega, Stanford, California 94305, United States
      More by Jeffrey B.-H. Tok
    • Harald Rupp
      Harald Rupp
      Macromolecular Chemistry, Division of Technical and Macromolecular Chemistry, Institute of Chemistry, Faculty of Natural Sciences II (Chemistry, Physics and Mathematics), Martin Luther University Halle-Wittenberg, von-Danckelmann-Platz 4, Halle D-06120, Germany
      More by Harald Rupp
      Orcidhttp://orcid.org/0000-0002-3309-706X
    • Wolfgang H. Binder
      Wolfgang H. Binder
      Macromolecular Chemistry, Division of Technical and Macromolecular Chemistry, Institute of Chemistry, Faculty of Natural Sciences II (Chemistry, Physics and Mathematics), Martin Luther University Halle-Wittenberg, von-Danckelmann-Platz 4, Halle D-06120, Germany
      More by Wolfgang H. Binder
      Orcidhttp://orcid.org/0000-0003-3834-5445
    • Zhenan Bao*
      Zhenan Bao
      Department of Chemical Engineering, Stanford University, 443 Via Ortega, Stanford, California 94305, United States
      *(Z.B.) Email: [email protected]
      More by Zhenan Bao
      Orcidhttp://orcid.org/0000-0002-0972-1715
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    ACS Applied Polymer Materials

    Cite this: ACS Appl. Polym. Mater. 2020, 2, 9, 4127–4139
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    https://doi.org/10.1021/acsapm.0c00755
    Published August 3, 2020
    Copyright © 2020 American Chemical Society
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    Abstract

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    We present a comprehensive investigation of mechanical properties of supramolecular polymer networks with rationally developed multistrength hydrogen-bonding interactions. Self-healing poly(dimethylsiloxane) (PDMS)-based elastomers with varying elasticity, fracture toughness, and the ability to dissipate strain energy through the reversible breakage and re-formation of the supramolecular interactions were obtained. By changing the ratio between isophorone diisocyanate (IU), 4,4′-methylenebis(cyclohexyl isocyanate) (MCU), and 4,4′-methylenebis(phenyl isocyanate) (MPU) and by varying the molecular weight of the PDMS precursor, we obtained a library of poly(urea)s to study the interplay of mechanical performance and self-healability. The Young’s moduli of the presented materials ranged between 0.4 and 13 MPa and increased with decreasing molecular weight of the PDMS precursor and increasing content of MCU or MPU units related to the formation of stronger hydrogen-bonding interactions. By exchanging MPU against MCU units, we achieved an optimum balance between mechanical properties and self-healing performance, and by the additional reduction of the molecular weight of the precursor polymer, a minimum recovery of 80% in stress within 12 h at room temperature was observed. Selected poly(urea)s could be processed via 3D printing by the conventional extrusion method, obtaining dimensionally stable and freestanding objects.

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    • Materials and instrumentation; Synthesis of PDMS-based elastomers using two diisocyanates: reaction scheme and material details; 1H NMR spectra of PDMS-3-IU1.0, PDMS-3-MPU0.4-IU0.6, PDMS-3-MCU1.0, PDMS-5-IU1.0, and PDMS-5-MCU1.0; SEC traces of the PDMS-3-MPU and the PDMS-3-MCU series; IR spectra of PDMS-3-IU1.0, PDMS-3-MPU0.4-IU0.6, PDMS-3-MCU1.0, PDMS-3-MPU1.0, PDMS-5-IU1.0, and PDMS-5-MCU1.0; ESI-ToF mass spectrum of PDMS-3-MCU0.2-IU0.8; thermal characterization, Young’s moduli and stress–strain-curves; self-healing efficiencies; cyclic stress–strain curves of PDMS-3-MPU0.4-IU0.6 and PDMS-3-MCU1.0; rheology investigations; viscosity vs shear rate investigations of PDMS-3-IU1.0 and PDMS-3-MPU0.4-IU0.6 (PDF)

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    ACS Applied Polymer Materials

    Cite this: ACS Appl. Polym. Mater. 2020, 2, 9, 4127–4139
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsapm.0c00755
    Published August 3, 2020
    Copyright © 2020 American Chemical Society
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