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Rapid Photothermal Healing of Vitrimer Nanocomposites Activated by Gold-Nanoparticle-Coated Graphene Nanoplatelets

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    Rapid Photothermal Healing of Vitrimer Nanocomposites Activated by Gold-Nanoparticle-Coated Graphene Nanoplatelets
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    • Yixin Ren
      Yixin Ren
      Materials and Manufacturing Directorate, Air Force Research Laboratory, Wright-Patterson Air Force Base, Ohio 45433, United States
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    • Amber M. Hubbard
      Amber M. Hubbard
      Materials and Manufacturing Directorate, Air Force Research Laboratory, Wright-Patterson Air Force Base, Ohio 45433, United States
      National Research Council Research Associate, Air Force Research Laboratory, Wright-Patterson Air Force Base, Ohio 45433, United States
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    • Drake Austin
      Drake Austin
      Materials and Manufacturing Directorate, Air Force Research Laboratory, Wright-Patterson Air Force Base, Ohio 45433, United States
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    • Jinghang Dai
      Jinghang Dai
      Sibley School of Mechanical and Aerospace Engineering, Cornell University, Ithaca, New York 14850, United States
      More by Jinghang Dai
      Orcidhttps://orcid.org/0000-0003-0215-7602
    • Chen Li
      Chen Li
      Sibley School of Mechanical and Aerospace Engineering, Cornell University, Ithaca, New York 14850, United States
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    • Renjiu Hu
      Renjiu Hu
      Sibley School of Mechanical and Aerospace Engineering, Cornell University, Ithaca, New York 14850, United States
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      Orcidhttps://orcid.org/0000-0003-4651-3349
    • Peter Papaioannou
      Peter Papaioannou
      Materials and Manufacturing Directorate, Air Force Research Laboratory, Wright-Patterson Air Force Base, Ohio 45433, United States
      Strategic Ohio Council for Higher Education (SOCHE) Program, Wright-Patterson Air Force Base, Ohio 45433, United States
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    • Catalin R. Picu
      Catalin R. Picu
      Department of Mechanical, Aerospace, and Nuclear Engineering, Rensselaer Polytechnic Institute, Troy, New York 12180, United States
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      Orcidhttps://orcid.org/0000-0001-8371-3564
    • Dominik Konkolewicz
      Dominik Konkolewicz
      Department of Chemistry and Biochemistry, Miami University, Oxford, Ohio 45056, United States
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      Orcidhttps://orcid.org/0000-0002-3828-5481
    • Alireza Sarvestani
      Alireza Sarvestani
      Department of Mechanical Engineering, Mercer University, Macon, Georgia 31207, United States
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      Orcidhttps://orcid.org/0000-0001-8762-7575
    • Nicholas Glavin
      Nicholas Glavin
      Materials and Manufacturing Directorate, Air Force Research Laboratory, Wright-Patterson Air Force Base, Ohio 45433, United States
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      Orcidhttps://orcid.org/0000-0002-9447-7509
    • Vikas Varshney
      Vikas Varshney
      Materials and Manufacturing Directorate, Air Force Research Laboratory, Wright-Patterson Air Force Base, Ohio 45433, United States
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      Orcidhttps://orcid.org/0000-0002-2613-458X
    • Ajit K. Roy
      Ajit K. Roy
      Materials and Manufacturing Directorate, Air Force Research Laboratory, Wright-Patterson Air Force Base, Ohio 45433, United States
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      Orcidhttps://orcid.org/0000-0002-3344-7437
    • Zhiting Tian
      Zhiting Tian
      Sibley School of Mechanical and Aerospace Engineering, Cornell University, Ithaca, New York 14850, United States
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      Orcidhttps://orcid.org/0000-0002-5098-7507
    • Dhriti Nepal*
      Dhriti Nepal
      Materials and Manufacturing Directorate, Air Force Research Laboratory, Wright-Patterson Air Force Base, Ohio 45433, United States
      *E-mail: [email protected]
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      Orcidhttps://orcid.org/0000-0002-0972-9960
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    ACS Applied Nano Materials

    Cite this: ACS Appl. Nano Mater. 2024, 7, 16, 18769–18778
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    https://doi.org/10.1021/acsanm.4c02190
    Published August 2, 2024
    Copyright © 2024 American Chemical Society
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    Abstract

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    Vitrimers, an emerging class of polymer materials, are thermosets with dynamic covalent cross-linkers, allowing for topology rearrangement at elevated temperatures. However, vitrimers have several drawbacks, such as slow response times and often lack photothermal catalytic activity. Herein, we demonstrate that embedding functional nanofillers, i.e., hierarchically assembled plasmonic gold nanoparticles (AuNPs) on graphene nanoplatelets (GNPIs) into a vitrimer matrix, induces an ultrafast photothermal healing response. Unlike previous research that mainly focused on bulk materials, our exploration of vitrimer nanocomposite films uncovers unique advantages, such as optical transparency in the visible wavelength, flexibility, and ultrafast localized healing upon exposure to a 532 nm wavelength laser. These remarkable properties of vitrimer nanocomposite films were demonstrated with three various filler compositions and concentrations, where AuNPs/GNPls serve as a powerful filler. Photothermally activated self-healing of these hybrid materials is demonstrated by taking advantage of the localized surface plasmon resonance (LSPR) of AuNPs and the broad absorbance wavelength and high thermal conductivity of GNPls. Furthermore, profilometry is utilized to quantify the volume percent recovery of healing, providing quantitative evidence of increased healing with a higher filler concentration and laser dosage. This localized, ultrafast healing is pivotal for future coating applications, where bulk heating could lead to undesirable deformations. Our comprehensive understanding of the role of filler composition, filler concentration, and laser dosage in the self-healing properties of films opens up a wide array of potential applications for these light-responsive functional materials. The potential applications of these materials span from self-healing coatings to flexible electronics, inspiring a new era of innovative solutions.

    Copyright © 2024 American Chemical Society

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    Supporting Information

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    Figure S1Figure S2Figure S3Figure S4Figure S5Figure S6Figure S7Figure S8Figure S9Figure S10Figure S11Figure S12Figure S13Figure S14Figure S15Figure S16Figure S17Figure S18The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsanm.4c02190

    • Scheme S1: Schematics showing (a) chemical structures of the reactants and catalyst, bisphenol A diglycidyl ether (DGEBA), sebacic Acid, and 1,5,7-triazabicyclo[4.4.0]dec-5-ene (TBD as a catalyst). (b) Chemical reactions showing acid and epoxy lead to an esterification reaction resulting in the growth of a polymeric chain (top) and transesterification reaction driven by the catalyst (bottom), the key mechanism for the dynamic reaction. Figure S1: FTIR confirms complete curing of the vitrimer material. Figure S2: Schematic diagrams depicting vitrimer synthesis where additional sonication and shear mixing are required for increased filler dispersion. Figure S3: Optical microscopy confirms increased filler dispersion with additional shear mixing and sonication via image analysis. Figure S4: HAADF-STEM and EDX confirm the presence of gold decorated on the graphene nanoplatelets. Figure S5. UV–visible spectroscopy (UV–vis) spectra show the evolution of transmission for three types of vitrimer nanocomposites at different weight percentages of filler content: (a) GNPIs, (b) AuNPs, and (c) AuNPs/GNPls. Figure S6: UV–vis is shown for all the vitrimer composites. Figure S7: TGA results are shown for all vitrimer nanocomposites. Figure S8: DSC results are shown for all the vitrimer nanocomposites. Tensile test results are shown for neat vitrimer and vitrimer nanocomposite films. Figure S9: Temperature sweep results from DMA are shown for all vitrimer composites. Figure S10: Nonisothermal creep is shown for increasing filler concentration. Figure S11: Schematic diagram depicting the laser apparatus utilized for all photothermal healing experiments. Figure S12: Profilometry scans are shown for vitrimer healing studies with a variety of filler compositions. Figure S13: Profilometry images and scans are shown to demonstrate the surface deformation as a result of thermal expansion. Figure S14: Schematic diagram of TTG set up. Figure S15: Measured TTG signal for the 0.2 wt % GNPl vitrimer nanocomposite film. Figure S16: In-plane thermal diffusivity measured from TTG of different vitrimer nanocomposite films. Figure S17: Representative tensile stress–strain curve of thin vitrimer films showing the influence of filler and dispersion quality influencing the mechanical properties. Figure S18: Summary of the tensile testing data of neat vitrimer and composite: (a) Modulus (GPa) and strain at break (%), and (b) toughness (MJ/m3) (PDF)

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    1. Patrick Schütz, Siraphat Weerathaworn, Clas Jürgensen, Birgit Hankiewicz, Volker Abetz. Nanocomposites from Au‐Doped Vinylogous Urethane Vitrimers Based on Different Block Copolymers and Their Recyclability in Combination with Plasmonic Heating. Macromolecular Rapid Communications 2025, 15 https://doi.org/10.1002/marc.202401027
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    ACS Applied Nano Materials

    Cite this: ACS Appl. Nano Mater. 2024, 7, 16, 18769–18778
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsanm.4c02190
    Published August 2, 2024
    Copyright © 2024 American Chemical Society
    Request reuse permissions

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