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

  • 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]
  • 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
  • Jeffrey B.-H. Tok
    Jeffrey B.-H. Tok
    Department of Chemical Engineering, Stanford University, 443 Via Ortega, Stanford, California 94305, United States
  • 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
  • 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
  • , and 
  • 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
Cite this: ACS Appl. Polym. Mater. 2020, 2, 9, 4127–4139
Publication Date (Web):August 3, 2020
https://doi.org/10.1021/acsapm.0c00755
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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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsapm.0c00755.

    • 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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