Chain and Segmental Dynamics in Polymer–Nanoparticle Composites with High Nanoparticle Loading

Lin, Emily Y.; Frischknecht, Amalie L.; Riggleman, Robert A.

doi:10.1021/acs.macromol.1c00206

Chain and Segmental Dynamics in Polymer–Nanoparticle Composites with High Nanoparticle Loading

Journal Article · Wed Jun 09 00:00:00 EDT 2021 · Macromolecules

DOI:https://doi.org/10.1021/acs.macromol.1c00206· OSTI ID:1810337

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Univ. of Pennsylvania, Philadelphia, PA (United States)
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Recent experimental and simulation studies have shown that polymer–nanoparticle (NP) composites (PNCs) with ultra-high NP loading (>50%) exhibit remarkable mechanical properties and dramatic increases in polymer glass-transition temperature, viscosity, and thermal stability compared to the bulk polymer. These deviations in macroscopic properties suggest a slowdown in both segmental and chain-scale polymer dynamics due to confinement. In this work, we examine the polymer conformations and dynamics in these PNCs using molecular dynamics simulations of both unentangled and entangled coarse-grained polymers in random-close-packed NP packings with varying polymer fill fractions. We find that the changes in the polymer dynamics depend on the number of NPs in contact with a polymer segment. Using the number of polymer–NP contacts and different polymer chain conformations as criteria for categorization, we further examine the polymer dynamics at multiple length scales to show the high level of dynamic heterogeneity in PNCs with ultra-high NP loading.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC04-94AL85000

OSTI ID:: 1810337

Report Number(s):: SAND--2021-7731J; 696974

Journal Information:: Macromolecules, Journal Name: Macromolecules Journal Issue: 12 Vol. 54; ISSN 0024-9297

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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