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Tuning the Properties of Nanocomposites by Trapping Them in Deep Metastable States

  • Zhengping Zhou*
    Zhengping Zhou
    Chemical Sciences Division, Physical Sciences Directorate, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    *Email: [email protected]
  • Vera Bocharova
    Vera Bocharova
    Chemical Sciences Division, Physical Sciences Directorate, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Rajeev Kumar
    Rajeev Kumar
    Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    More by Rajeev Kumar
  • Anne-Caroline Genix
    Anne-Caroline Genix
    Laboratoire Charles Coulomb, Université de Montpellier, CNRS, Montpellier F-34095, France
  • Bobby Carroll
    Bobby Carroll
    Department of Chemistry, University of Tennessee, Knoxville, Tennessee 37996, United States
  • Subarna Samanta
    Subarna Samanta
    Department of Chemistry, University of Tennessee, Knoxville, Tennessee 37996, United States
  • Ivan Popov
    Ivan Popov
    Chemical Sciences Division, Physical Sciences Directorate, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    More by Ivan Popov
  • Amanda Young-Gonzales
    Amanda Young-Gonzales
    Department of Chemistry, University of Tennessee, Knoxville, Tennessee 37996, United States
  • Alexander Kisliuk
    Alexander Kisliuk
    Chemical Sciences Division, Physical Sciences Directorate, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Seung Pyo Jeong
    Seung Pyo Jeong
    Chemical Sciences Division, Physical Sciences Directorate, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Jan Ilavsky
    Jan Ilavsky
    Advanced Photon Source, Argonne National Laboratory, Argonne, Illinois 60439, United States
    More by Jan Ilavsky
  • , and 
  • Alexei P. Sokolov*
    Alexei P. Sokolov
    Chemical Sciences Division, Physical Sciences Directorate, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    Department of Chemistry, University of Tennessee, Knoxville, Tennessee 37996, United States
    *Email: [email protected]
Cite this: ACS Appl. Polym. Mater. 2022, 4, 5, 3174–3182
Publication Date (Web):April 12, 2022
https://doi.org/10.1021/acsapm.1c01623
Copyright © 2022 American Chemical Society

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    Abstract

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    The interfacial region formed in a polymer matrix around nanoparticles (NPs) controls many macroscopic properties of polymer nanocomposites (PNCs). However, understanding the factors controlling the structure and properties of the interfacial region remains a challenge. We demonstrated that the initial trapping of polymer chains at surfaces of NPs in solution strongly affects the macroscopic properties of PNCs. The most surprising result is that the differences in properties of PNCs persist even after an extremely long thermal annealing time. We ascribe the observed changes to the formation of an interfacial layer that is trapped in a deep metastable state already in solution. Furthermore, the presented analysis suggests that the PNC equilibration time is defined by the chain desorption time that can be extremely long and, in some cases, even not accessible on a reasonable experimental time scale. These results highlight the importance of polymer solution concentrations on the formation of an interfacial layer and the macroscopic properties of PNCs.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsapm.1c01623.

    • Calculation of the radius of gyration (Rg) and critical concentration (C*); calculation of the distance between SiO2 NPs in solution; analysis of BDS spectra using ILM; estimate of mechanical properties using mechanical TPM and ILM; PCS results; ICFs; characteristics of SiO2 NPs and PNCs in solution; DSC analysis; reversing heat capacity and its derivative; representative plot of the LM from BLS; segmental relaxation; volume fraction of the interfacial region presented as a function of polymer concentration; SCFT calculations; SCFT parameters for simulating the adsorption of P2VP chains from ethanol onto a single spherical nanoparticle; segment and solvent density profile; density profiles of loops, tails, and free segments near the spherical nanoparticle; segment and solvent density profiles for various strengths of the segment–solvent interaction parameter; additional thermogravimetric data and kinetic study data; comparison of the dielectric loss spectra; annealing time dependence of the segmental relaxation times and conductivity; USAXS data; analytical estimates of polymer adsorption onto a spherical nanoparticle; and the effect of segment–nanoparticle interaction energy strength on the number of adsorbed monomers of a chain (PDF)

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    Cited By

    This article is cited by 2 publications.

    1. Wenzhi Cui, Wei You, Wei Yu. Interplay of Grafted and Adsorbed Chains at the Polymer–Particle Interface in Tuning the Mechanical Reinforcement in Polymer Nanocomposites. ACS Applied Polymer Materials 2024, 6 (3) , 1843-1852. https://doi.org/10.1021/acsapm.3c02700
    2. Mayank Jhalaria, Andrew M. Jimenez, Reha Mathur, Marshall C. Tekell, Yucheng Huang, Suresh Narayanan, Brian C. Benicewicz, Sanat K. Kumar. Long-Term Aging in Miscible Polymer Nanocomposites. Macromolecules 2022, 55 (11) , 4502-4515. https://doi.org/10.1021/acs.macromol.2c00332

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