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Addition of Short Polymer Chains Mechanically Reinforces Glassy Poly(2-vinylpyridine)–Silica Nanoparticle Nanocomposites

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    Addition of Short Polymer Chains Mechanically Reinforces Glassy Poly(2-vinylpyridine)–Silica Nanoparticle Nanocomposites
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    • Vera Bocharova*
      Vera Bocharova
      Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
      *(V.B.) Email [email protected]
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      Orcidhttp://orcid.org/0000-0003-4270-3866
    • Anne-Caroline Genix
      Anne-Caroline Genix
      Laboratoire Charles Coulomb (L2C), Université de Montpellier, CNRS, F-34095 Montpellier, France
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    • Jan-Michael Y. Carrillo*
      Jan-Michael Y. Carrillo
      Computational Sciences and Engineering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
      Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
      *(J.-M.Y.C.) Email [email protected]
      More by Jan-Michael Y. Carrillo
      Orcidhttp://orcid.org/0000-0001-8774-697X
    • Rajeev Kumar*
      Rajeev Kumar
      Computational Sciences and Engineering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
      Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
      *(R.K.) Email [email protected]
      More by Rajeev Kumar
      Orcidhttp://orcid.org/0000-0001-9494-3488
    • Bobby Carroll
      Bobby Carroll
      Department of Physics, University of Tennessee, Knoxville, Tennessee 37996, United States
      More by Bobby Carroll
      Orcidhttp://orcid.org/0000-0002-0536-9734
    • Andrew Erwin
      Andrew Erwin
      Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
      School of Material Science and Engineering, Georgia Tech, Atlanta, Georgia 30332, United States
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    • Dmitry Voylov
      Dmitry Voylov
      Department of Physics, University of Tennessee, Knoxville, Tennessee 37996, United States
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      Orcidhttp://orcid.org/0000-0001-5552-6024
    • Alexander Kisliuk
      Alexander Kisliuk
      Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
      More by Alexander Kisliuk
    • Yangyang Wang
      Yangyang Wang
      Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
      More by Yangyang Wang
      Orcidhttp://orcid.org/0000-0001-7042-9804
    • Bobby G. Sumpter
      Bobby G. Sumpter
      Computational Sciences and Engineering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
      Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
      More by Bobby G. Sumpter
      Orcidhttp://orcid.org/0000-0001-6341-0355
    • Alexei P. Sokolov
      Alexei P. Sokolov
      Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
      Department of Physics, University of Tennessee, Knoxville, Tennessee 37996, United States
      Department of Chemistry, University of Tennessee, Knoxville, Tennessee 37996, United States
      More by Alexei P. Sokolov
      Orcidhttp://orcid.org/0000-0002-8187-9445
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    ACS Applied Nano Materials

    Cite this: ACS Appl. Nano Mater. 2020, 3, 4, 3427–3438
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsanm.0c00180
    Published March 23, 2020
    Copyright © 2020 American Chemical Society
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    Abstract

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    The addition of hard fillers to a polymer matrix is a well-known process for achieving mechanical reinforcement. With a decrease in the size of the fillers, the contribution from polymer–particle nanometer-sized interfaces becomes significant, and these interfaces affect the mechanical performance of polymer nanocomposites (PNCs) beyond the limits established for conventional composites. However, the molecular mechanisms underlying the improvement in the mechanical performance of glassy PNCs remain unresolved, necessitating a deeper understanding of the structure–property relationships in these intrinsically heterogeneous systems. In this effort, by using Brillouin light scattering (BLS) and dynamic mechanical analysis (DMA), we demonstrated that adding shorter chains to a PNC prepared with high molecular weight polymers significantly improved the mechanical properties of the PNC in the glassy state. The strongest enhancement of mechanical properties occurred at an optimum concentration of short chains. This is in contrast to the behavior of the glass transition temperature of PNCs which shows a monotonic decrease with an increase in the concentration of shorter chains. Using experimental data and coarse-grained molecular dynamics (MD) simulations, we have identified the molecular mechanism leading to the observed nonmonotonic changes in mechanical reinforcement. This mechanism includes changes in the nanoscale organization at the interface combined with chain stretching amplified by the addition of the short chains. Overall, our approach paves a simple and cost-effective pathway to fabricating glassy PNCs with significantly improved mechanical properties that will fill various practical needs.

    Copyright © 2020 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/acsanm.0c00180.

    • Additional information about characterization of PNCs with DSC, DMA, BDS, SAXS, and details of MD simulations (PDF)

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    Cited By

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    This article is cited by 26 publications.

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    ACS Applied Nano Materials

    Cite this: ACS Appl. Nano Mater. 2020, 3, 4, 3427–3438
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsanm.0c00180
    Published March 23, 2020
    Copyright © 2020 American Chemical Society
    Request reuse permissions

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