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Influence of the Bound Polymer Layer on Nanoparticle Diffusion in Polymer Melts

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Department of Materials Science and Engineering, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States
Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
§ Department of Physics, University of Sheffield, Sheffield, S3 7RH, United Kingdom
Department of Materials Science and Engineering, University of Illinois, Urbana, Illinois 61801, United States
Cite this: ACS Macro Lett. 2016, 5, 10, 1141–1145
Publication Date (Web):September 23, 2016
Copyright © 2016 American Chemical Society

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    We measure the center-of-mass diffusion of silica nanoparticles (NPs) in entangled poly(2-vinylpyridine) (P2VP) melts using Rutherford backscattering spectrometry. While these NPs are well within the size regime where enhanced, nonhydrodynamic NP transport is theoretically predicted and has been observed experimentally (2RNP/dtube ≈ 3, where 2RNP is the NP diameter and dtube is the tube diameter), we find that the diffusion of these NPs in P2VP is in fact well-described by the hydrodynamic Stokes–Einstein relation. The effective NP diameter 2Reff is significantly larger than 2RNP and strongly dependent on P2VP molecular weight, consistent with the presence of a bound polymer layer on the NP surface with thickness heff ≈ 1.1Rg. Our results show that the bound polymer layer significantly augments the NP hydrodynamic size in polymer melts with attractive polymer–NP interactions and effectively transitions the mechanism of NP diffusion from the nonhydrodynamic to hydrodynamic regime, particularly at high molecular weights where NP transport is expected to be notably enhanced. Furthermore, these results provide the first experimental demonstration that hydrodynamic NP transport in polymer melts requires particles of size ≳5dtube, consistent with recent theoretical predictions.

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