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

Bocharova, Vera; Genix, Anne-Caroline; Carrillo, Jan-Michael Y.; Kumar, Rajeev; Carroll, Bobby; Erwin, Andrew; Voylov, Dmitry; Kisliuk, Alexander; Wang, Yangyang; Sumpter, Bobby G.; Sokolov, Alexei P.

doi:10.1021/acsanm.0c00180

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

Journal Article · Mon Mar 23 00:00:00 EDT 2020 · ACS Applied Nano Materials

DOI:https://doi.org/10.1021/acsanm.0c00180· OSTI ID:1608195

^[1]; Genix, Anne-Caroline ^[2]; ^[1]; ^[1]; ^[3]; Erwin, Andrew ^[4]; ^[3]; Kisliuk, Alexander ^[1]; ^[1]; ^[1]; ^[5]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. de Montpellier (France)
Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Georgia Tech, Atlanta, GA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

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 become 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 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 non-monotonic changes in mechanical reinforcement. Here, 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, cost-effective pathway to fabricating glassy PNCs with significantly improved mechanical properties that will fill various practical needs.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1608195

Journal Information:: ACS Applied Nano Materials, Journal Name: ACS Applied Nano Materials Journal Issue: 4 Vol. 3; ISSN 2574-0970

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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

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