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Title: Chain dynamics and nanoparticle motion in attractive polymer nanocomposites subjected to large deformations

Abstract

The effect of large deformation on the chain dynamics in attractive polymer nanocomposites was investigated using neutron scattering techniques. Quasielastic neutron backscattering measurements reveal a substantial reduction of polymer mobility in the presence of attractive, well-dispersed nanoparticles. Additionally, large deformations are observed to cause a further slowing down of the Rouse rates at high particle loadings, where the interparticle spacings are slightly smaller than the chain dimensions, i.e. in the strongly confined state. No noticeable change, however, was observed for a lightly confined system. The reptation tube diameter, measured by neutron spin echo, remained unchanged after shear, suggesting that the level of chain-chain entanglements is not significantly affected. The shearinduced changes in the interparticle bridging reflects on the slow nanoparticle motion measured by X-ray photon correlation spectroscopy. These results provide a first step for understanding how large shear can significantly affect the segmental motion in nanocomposites and open up new opportunities for designing mechanically responsive soft materials.

Authors:
ORCiD logo [1];  [1];  [2];  [3];  [4]
  1. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Center for Neutron Research; Univ. of Maryland, College Park, MD (United States)
  2. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Center for Neutron Research
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Science Foundation (NSF); USDOE Office of Science (SC)
OSTI Identifier:
1427470
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Soft Matter
Additional Journal Information:
Journal Volume: 13; Journal Issue: 43; Journal ID: ISSN 1744-683X
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Senses, Erkan, Tyagi, Madhusudan, Natarajan, Bharath, Narayanan, Suresh, and Faraone, Antonio. Chain dynamics and nanoparticle motion in attractive polymer nanocomposites subjected to large deformations. United States: N. p., 2017. Web. doi:10.1039/C7SM01009E.
Senses, Erkan, Tyagi, Madhusudan, Natarajan, Bharath, Narayanan, Suresh, & Faraone, Antonio. Chain dynamics and nanoparticle motion in attractive polymer nanocomposites subjected to large deformations. United States. https://doi.org/10.1039/C7SM01009E
Senses, Erkan, Tyagi, Madhusudan, Natarajan, Bharath, Narayanan, Suresh, and Faraone, Antonio. Thu . "Chain dynamics and nanoparticle motion in attractive polymer nanocomposites subjected to large deformations". United States. https://doi.org/10.1039/C7SM01009E. https://www.osti.gov/servlets/purl/1427470.
@article{osti_1427470,
title = {Chain dynamics and nanoparticle motion in attractive polymer nanocomposites subjected to large deformations},
author = {Senses, Erkan and Tyagi, Madhusudan and Natarajan, Bharath and Narayanan, Suresh and Faraone, Antonio},
abstractNote = {The effect of large deformation on the chain dynamics in attractive polymer nanocomposites was investigated using neutron scattering techniques. Quasielastic neutron backscattering measurements reveal a substantial reduction of polymer mobility in the presence of attractive, well-dispersed nanoparticles. Additionally, large deformations are observed to cause a further slowing down of the Rouse rates at high particle loadings, where the interparticle spacings are slightly smaller than the chain dimensions, i.e. in the strongly confined state. No noticeable change, however, was observed for a lightly confined system. The reptation tube diameter, measured by neutron spin echo, remained unchanged after shear, suggesting that the level of chain-chain entanglements is not significantly affected. The shearinduced changes in the interparticle bridging reflects on the slow nanoparticle motion measured by X-ray photon correlation spectroscopy. These results provide a first step for understanding how large shear can significantly affect the segmental motion in nanocomposites and open up new opportunities for designing mechanically responsive soft materials.},
doi = {10.1039/C7SM01009E},
journal = {Soft Matter},
number = 43,
volume = 13,
place = {United States},
year = {Thu Sep 28 00:00:00 EDT 2017},
month = {Thu Sep 28 00:00:00 EDT 2017}
}

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Works referenced in this record:

50th Anniversary Perspective : Are Polymer Nanocomposites Practical for Applications?
journal, January 2017


Single Chain Dynamic Structure Factor of Linear Polymers in an All-Polymer Nano-Composite
journal, March 2016


Conformation of Polymer Brushes under Shear: Chain Tilting and Stretching
journal, January 1996

  • Miao, Ling; Guo, Hong; Zuckermann, Martin J.
  • Macromolecules, Vol. 29, Issue 6
  • DOI: 10.1021/ma951071z

Segmental Dynamics of Polymer Melts with Spherical Nanoparticles
journal, July 2014

  • Gong, Shushan; Chen, Quan; Moll, Joseph F.
  • ACS Macro Letters, Vol. 3, Issue 8
  • DOI: 10.1021/mz500252f

Origin of Small-Angle Scattering from Contrast-Matched Nanoparticles: A Study of Chain and Filler Structure in Polymer Nanocomposites
journal, September 2015


Mechanical Reinforcement of Polymer Nanocomposites from Percolation of a Nanoparticle Network
journal, March 2015


Microscopic Chain Motion in Polymer Nanocomposites with Dynamically Asymmetric Interphases
journal, July 2016

  • Senses, Erkan; Faraone, Antonio; Akcora, Pinar
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep29326

Nanostructures and Dynamics of Macromolecules Bound to Attractive Filler Surfaces
journal, July 2015


Statistics of polymer adsorption under shear flow
journal, March 2010

  • He, Gui-Li; Messina, René; Löwen, Hartmut
  • The Journal of Chemical Physics, Vol. 132, Issue 12
  • DOI: 10.1063/1.3361673

Microscopic Dynamics of Polyethylene Glycol Chains Interacting with Silica Nanoparticles
journal, April 2013


Nanoparticle Motion within Glassy Polymer Melts
journal, February 2009


Structure and dynamics of polymer nanocomposites studied by X-ray and neutron scattering techniques
journal, August 2015

  • Genix, Anne-Caroline; Oberdisse, Julian
  • Current Opinion in Colloid & Interface Science, Vol. 20, Issue 4
  • DOI: 10.1016/j.cocis.2015.10.002

Dispersing Grafted Nanoparticle Assemblies into Polymer Melts through Flow Fields
journal, November 2013

  • Moll, Joseph; Kumar, Sanat K.; Snijkers, Frank
  • ACS Macro Letters, Vol. 2, Issue 12
  • DOI: 10.1021/mz400447k

Influence of the Bound Polymer Layer on Nanoparticle Diffusion in Polymer Melts
journal, September 2016


Rheology of Confined Polymer Melts under Shear Flow: Weak Adsorption Limit
journal, May 1995

  • Subbotin, A.; Semenov, A.; Hadziioannou, G.
  • Macromolecules, Vol. 28, Issue 11
  • DOI: 10.1021/ma00115a022

Anomalous structural and dynamical phase transitions of soft colloidal binary mixtures
journal, January 2012

  • Kandar, A. K.; Basu, J. K.; Narayanan, S.
  • Soft Matter, Vol. 8, Issue 39
  • DOI: 10.1039/c2sm25774b

Bound Polymer Layer in Nanocomposites
journal, April 2013

  • Jouault, Nicolas; Moll, Joseph F.; Meng, Dong
  • ACS Macro Letters, Vol. 2, Issue 5
  • DOI: 10.1021/mz300646a

Mechanistic model for deformation of polymer nanocomposite melts under large amplitude shear
journal, January 2013

  • Senses, Erkan; Akcora, Pinar
  • Journal of Polymer Science Part B: Polymer Physics, Vol. 51, Issue 9
  • DOI: 10.1002/polb.23247

Polymer Chain Dynamics in a Random Environment: Heterogeneous Mobilities
journal, April 2007


An Interface-Driven Stiffening Mechanism in Polymer Nanocomposites
journal, February 2013

  • Senses, Erkan; Akcora, Pinar
  • Macromolecules, Vol. 46, Issue 5
  • DOI: 10.1021/ma302275f

Small Particle Driven Chain Disentanglements in Polymer Nanocomposites
journal, April 2017


Structure and Entanglement Factors on Dynamics of Polymer-Grafted Nanoparticles
journal, April 2016


DAVE: A Comprehensive Software Suite for the Reduction, Visualization, and Analysis of Low Energy Neutron Spectroscopic Data
journal, November 2009

  • Azuah, Richard Tumanjong; Kneller, Larry R.; Qiu, Yiming
  • Journal of Research of the National Institute of Standards and Technology, Vol. 114, Issue 6
  • DOI: 10.6028/jres.114.025

Multiscale Dynamics of Polymers in Particle-Rich Nanocomposites
journal, July 2016


Conformations of Silica−Poly(ethylene−propylene) Nanocomposites
journal, December 2010

  • Nusser, Klaus; Neueder, Susanne; Schneider, Gerald J.
  • Macromolecules, Vol. 43, Issue 23
  • DOI: 10.1021/ma101898c

Rheology of Confined Polymer Melts under Shear Flow: Strong Adsorption Limit
journal, September 1995

  • Subbotin, A.; Semenov, A.; Manias, E.
  • Macromolecules, Vol. 28, Issue 5
  • DOI: 10.1021/ma00109a024

Neutron Spin Echo in Polymer Systems
book, January 2005

  • Richter, Dieter; Monkenbusch, Michael; Arbe, Arantxa
  • DOI: 10.1007/b106578

Network dynamics in nanofilled polymers
journal, April 2016

  • Baeza, Guilhem P.; Dessi, Claudia; Costanzo, Salvatore
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms11368

Modulating interfacial attraction of polymer-grafted nanoparticles in melts under shear
journal, January 2014

  • Senses, Erkan; Jiao, Yang; Akcora, Pinar
  • Soft Matter, Vol. 10, Issue 25
  • DOI: 10.1039/C4SM00460D

The high-flux backscattering spectrometer at the NIST Center for Neutron Research
journal, May 2003

  • Meyer, A.; Dimeo, R. M.; Gehring, P. M.
  • Review of Scientific Instruments, Vol. 74, Issue 5
  • DOI: 10.1063/1.1568557

A Microscopic Model for the Reinforcement and the Nonlinear Behavior of Filled Elastomers and Thermoplastic Elastomers (Payne and Mullins Effects)
journal, November 2008

  • Merabia, Samy; Sotta, Paul; Long, Didier R.
  • Macromolecules, Vol. 41, Issue 21
  • DOI: 10.1021/ma8014728

Effect of Nanoconfinement on Polymer Dynamics: Surface Layers and Interphases
journal, March 2013


Reversible Thermal Stiffening in Polymer Nanocomposites
journal, June 2015

  • Senses, Erkan; Isherwood, Andrew; Akcora, Pinar
  • ACS Applied Materials & Interfaces, Vol. 7, Issue 27
  • DOI: 10.1021/acsami.5b02046

Unexpected Molecular Weight Effect in Polymer Nanocomposites
journal, January 2016


Reinforcement Mechanism of Nanofilled Polymer Melts As Elucidated by Nonlinear Viscoelastic Behavior
journal, September 2002

  • Sternstein, S. S.; Zhu, Ai-Jun
  • Macromolecules, Vol. 35, Issue 19
  • DOI: 10.1021/ma020482u

Tailoring the alignment of string-like nanoparticle assemblies in a functionalized polymer matrix via steady shear
journal, January 2017


Interfaces and interphases in multicomponent materials: past, present, future
journal, April 2005


Reptation of a Polymer Chain in the Presence of Fixed Obstacles
journal, July 1971

  • de Gennes, P. G.
  • The Journal of Chemical Physics, Vol. 55, Issue 2
  • DOI: 10.1063/1.1675789

Chain Dynamics and Viscoelastic Properties of Poly(ethylene oxide)
journal, July 2008

  • Niedzwiedz, K.; Wischnewski, A.; Pyckhout-Hintzen, W.
  • Macromolecules, Vol. 41, Issue 13
  • DOI: 10.1021/ma800446n

Immobilized Polymer Layers on Spherical Nanoparticles
journal, April 2010

  • Harton, Shane E.; Kumar, Sanat K.; Yang, Hoichang
  • Macromolecules, Vol. 43, Issue 7
  • DOI: 10.1021/ma902484d

Modeling of Intermediate Structures and Chain Conformation in Silica–Latex Nanocomposites Observed by SANS During Annealing
journal, January 2012

  • Genix, Anne-Caroline; Tatou, Mouna; Imaz, Ainara
  • Macromolecules, Vol. 45, Issue 3
  • DOI: 10.1021/ma202308c

Study of the dynamics of poly(ethylene oxide) by combining molecular dynamic simulations and neutron scattering experiments
journal, March 2009

  • Brodeck, M.; Alvarez, F.; Arbe, A.
  • The Journal of Chemical Physics, Vol. 130, Issue 9
  • DOI: 10.1063/1.3077858

Entanglement-Controlled Subdiffusion of Nanoparticles within Concentrated Polymer Solutions
journal, August 2012


Chain Conformations and Bound-Layer Correlations in Polymer Nanocomposites
journal, March 2007


Dynamics at the Polymer/Nanoparticle Interface in Poly(2-vinylpyridine)/Silica Nanocomposites
journal, February 2014

  • Holt, Adam P.; Griffin, Philip J.; Bocharova, Vera
  • Macromolecules, Vol. 47, Issue 5
  • DOI: 10.1021/ma5000317

Network dynamics in nanofilled polymers
text, January 2016

  • K., Kumar, Sanat; Shushan, Gong,; P., Baeza, Guilhem
  • The University of North Carolina at Chapel Hill University Libraries
  • DOI: 10.17615/wpjw-0671

Works referencing / citing this record:

Study of segmental dynamics and ion transport in polymer–ceramic composite electrolytes by quasi-elastic neutron scattering
journal, January 2019

  • Chen, X. Chelsea; Sacci, Robert L.; Osti, Naresh C.
  • Molecular Systems Design & Engineering, Vol. 4, Issue 2
  • DOI: 10.1039/c8me00113h

Anisotropic and heterogeneous dynamics in stretched elastomer nanocomposites
journal, January 2019

  • Ehrburger-Dolle, Françoise; Morfin, Isabelle; Bley, Françoise
  • Soft Matter, Vol. 15, Issue 18
  • DOI: 10.1039/c8sm02289e

Polymer dynamics under confinement
journal, January 2019

  • Richter, Dieter; Kruteva, Margarita
  • Soft Matter, Vol. 15, Issue 37
  • DOI: 10.1039/c9sm01141b