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Diffusion of Sticky Nanoparticles in a Polymer Melt: Crossover from Suppressed to Enhanced Transport

Carroll, Bobby and Bocharova, Vera and Carrillo, Jan-Michael Y. and Kisliuk, Alexander and Cheng, Shiwang and Yamamoto, Umi and Schweizer, Kenneth S. and Sumpter, Bobby G. and Sokolov, Alexei P. (2018) Diffusion of Sticky Nanoparticles in a Polymer Melt: Crossover from Suppressed to Enhanced Transport. Macromolecules, 51 (6). pp. 2268-2275. ISSN 0024-9297. https://resolver.caltech.edu/CaltechAUTHORS:20180418-103622719

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Abstract

The self-diffusion of a single large particle in a fluid is usually described by the classic Stokes–Einstein (SE) hydrodynamic relation. However, there are many fluids where the SE prediction for nanoparticles diffusion fails. These systems include diffusion of nanoparticles in porous media, in entangled and unentangled polymer melts and solutions, and protein diffusion in biological environments. A fundamental understanding of the microscopic parameters that govern nanoparticle diffusion is relevant to a wide range of applications. In this work, we present experimental measurements of the tracer diffusion coefficient of small and large nanoparticles that experience strong attractions with unentangled and entangled polymer melt matrices. For the small nanoparticle system, a crossover from suppressed to enhanced diffusion is observed with increasing polymer molecular weight. We interpret these observations based on our theoretical and simulation insights of the preceding article (paper 1) as a result of a crossover from an effective hydrodynamic core–shell to a nonhydrodynamic vehicle mechanism of transport, with the latter strongly dependent on polymer–nanoparticle desorption time. A general zeroth-order qualitative picture for small sticky nanoparticle diffusion in polymer melts is proposed.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/acs.macromol.7b02695DOIArticle
ORCID:
AuthorORCID
Carroll, Bobby0000-0002-0536-9734
Bocharova, Vera0000-0003-4270-3866
Carrillo, Jan-Michael Y.0000-0001-8774-697X
Cheng, Shiwang0000-0001-7396-4407
Sumpter, Bobby G.0000-0001-6341-0355
Additional Information:© 2018 American Chemical Society. Received: December 19, 2017. Revised: February 14, 2018. Published: March 9, 2018. This work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division. Simulations were performed at the Center for Nanophase Materials Sciences, which is a US Department of Energy Office of Science User Facility. This research also used resources of the Oak Ridge Leadership Computing Facility at Oak Ridge National Laboratory, which is supported by the Office of Science of the Department of Energy under Contract DE-AC05-00OR22725. The authors declare no competing financial interest.
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-AC05-00OR22725
Issue or Number:6
Record Number:CaltechAUTHORS:20180418-103622719
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20180418-103622719
Official Citation:Diffusion of Sticky Nanoparticles in a Polymer Melt: Crossover from Suppressed to Enhanced Transport Bobby Carroll, Vera Bocharova, Jan-Michael Y. Carrillo, Alexander Kisliuk, Shiwang Cheng, Umi Yamamoto, Kenneth S. Schweizer, Bobby G. Sumpter, and Alexei P. Sokolov Macromolecules 2018 51 (6), 2268-2275 DOI: 10.1021/acs.macromol.7b02695
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:85944
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:18 Apr 2018 20:51
Last Modified:03 Oct 2019 19:37

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