Multiscale Dynamics of Polymers in Particle-Rich Nanocomposites

Mangal, Rahul; Wen, Yu Ho; Choudhury, Snehashis; Archer, Lynden A.

doi:10.1021/acs.macromol.6b00496

Title: Multiscale Dynamics of Polymers in Particle-Rich Nanocomposites

Journal Article · Thu Jul 14 00:00:00 EDT 2016 · Macromolecules

DOI:https://doi.org/10.1021/acs.macromol.6b00496· OSTI ID:1327063

Mangal, Rahul ^[1]; Wen, Yu Ho ^[1]; Choudhury, Snehashis ^[1]; Archer, Lynden A. ^[1]

Cornell Univ., Ithaca, NY (United States)

In this paper we report on the dynamics of entangled polymers in polymer–nanoparticle composites (PNCs) with moderate and high particle loadings. Using composites comprised of poly(ethylene glycol) (PEG)-tethered silica (SiO₂) nanoparticles and poly(methyl methacrylate) (PMMA), we show by means of small-angle X-ray scattering (SAXS) analysis that the nanoparticles are uniformly dispersed over a range of particle concentrations. From oscillatory shear rheology measurements, we find that the time–temperature superposition (TTS) principle holds for these SiO₂-PEG/PMMA PNCs up to a particle concentration Φ_G ≈ 11% where the materials begin to exhibit soft glassy rheological properties. At particle concentrations below Φ_G, we take advantage of TTS to create dynamic maps for PNCs that span time scales ranging from fast segmental motions to slow terminal relaxation of polymer chains. These maps reveal that at low Φ and depending on the host polymer (PMMA) molecular weight (M_w), hairy nanoparticles may either speed up or slow down terminal relaxation of the host. In contrast, at high Φ, nanoparticles slow down polymer dynamics on intermediate and long time scales, irrespective of the host polymer M_w. The slowdown coincides with particle concentrations at which the mean interparticle spacing lies below the equilibrium tube diameter of the entangled PMMA host and is thought to reflect the onset of confinement dynamics of polymer chains in PNCs. Studies of PNCs in the confinement regime reveal important analogies between glassy attributes of 3D-confined polymer chains in nanocomposites with those of polymer thin films supported on attractive substrates.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: National Science Foundation (NSF)

Grant/Contract Number:: CBET-1512297; AC02-06CH11357

OSTI ID:: 1327063

Journal Information:: Macromolecules, Vol. 49, Issue 14; ISSN 0024-9297

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: ENGLISH

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Cited by: 25 works

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