Polymer Chain Diffusion in All-Polymer Nanocomposites: Confinement vs Chain Acceleration

Rostom, Sahar; White, B. Tyler; Yuan, Guangcui; Saito, Tomonori; Dadmun, Mark D.

doi:10.1021/acs.jpcc.0c06022

Polymer Chain Diffusion in All-Polymer Nanocomposites: Confinement vs Chain Acceleration

Journal Article · Wed Jul 29 00:00:00 EDT 2020 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.0c06022· OSTI ID:1840214

Rostom, Sahar ^[1]; ^[2]; Yuan, Guangcui ^[3]; ^[2]; ^[4]

Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Center for Neutron Research; Georgetown Univ., Washington, DC (United States)
Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

All-polymer nanocomposites, in which soft, polymer-based nanoparticles are dispersed in the polymer matrix, have received great interest lately due to their potential use in a range of applications, including drug delivery and self-healing materials. However, the impact of this new class of nanoparticles on the dynamics of a linear polymer matrix in an all-polymer nanocomposite is still largely unknown. In this work, we report that the addition of polystyrene soft nanoparticles accelerates the diffusion of high molecular weight linear PS chains over a range of nanoparticle loadings. Our results show that at nanoparticle loadings below 1%, the diffusion of the linear matrix increases, presumably via a constraint release mechanism. At loadings above 1%, the increase in diffusion is mitigated by confinement effects of the nanoparticles. Thus, the response of these all-polymer nanocomposites is dominated by the balance of entropic confinement of the chain, which slows diffusion and a constraint release mechanism that speeds up the diffusion. However, the diffusion of the linear chain in the all-polymer nanocomposite is faster than that of the same chain in the melt at all loadings, diverging from the behavior of most nanocomposites with hard, impenetrable nanoparticles. Thus, the mechanism that accelerates the chain diffusion dominates in these systems. This behavior is unusual and fundamentally different than what has been reported for nanocomposites with hard inorganic nanoparticles, indicating that new perspectives are needed for these materials where the control of loading can either accelerate or decelerate the dynamics of the matrix in a distinctive manner.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1840214

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 34 Vol. 124; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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