A multiple length scale description of the mechanism of elastomer stretching
Abstract
Conventionally, the stretching of rubber is modeled exclusively by rotations of segments of the embedded polymer chains; i.e. changes in entropy. However models have not been tested on all relevant length scales due to a lack of appropriate probes. Here we present a universal X-ray based method for providing data on the structure of rubbers in the 2–50 Å range. First results relate to the elongation of a silicone rubber. We identify several non-entropic contributions to the free energy and describe the associated structural changes. By far the largest contribution comes from structural changes within the individual monomers, but among the contributions is also an elastic strain, acting between chains, which is 3–4 orders of magnitude smaller than the macroscopic strain, and of the opposite sign, i.e. extension of polymer chains in the direction perpendicular to the stretch. We find this may be due to trapped entanglements relaxing to positions close to the covalent crosslinks.
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical and Engineering Materials Division
- Technical Univ. of Denmark, Lyngby (Denmark). Danish Polymer Centre, Dept. of Chemical Engineering
- Univ. of New South Wales, Sydney, NSW (Australia). School of Materials Science and Engineering; European Synchrotron Radiation Facility (ESRF), Grenoble (France)
- European Synchrotron Radiation Facility (ESRF), Grenoble (France)
- Roskilde Univ., Roskilde (Denmark). Dept. of Sciences, Glass and Time
- Technical Univ. of Denmark, Lyngby (Denmark). Dept. of Physics, Neutrons and X-rays for Materials Physics
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); Danish National Research Foundation; Danish Natural Science Research Council
- OSTI Identifier:
- 1328263
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- RSC Advances
- Additional Journal Information:
- Journal Volume: 6; Journal Issue: 98; Journal ID: ISSN 2046-2069
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Neuefeind, Joerg C., Skov, Anne L., Daniels, John E., Honkimaeki, Veijo, Jakobsen, Bo, Oddershede, Jette, and Poulsen, Henning F. A multiple length scale description of the mechanism of elastomer stretching. United States: N. p., 2016.
Web. doi:10.1039/c6ra22802j.
Neuefeind, Joerg C., Skov, Anne L., Daniels, John E., Honkimaeki, Veijo, Jakobsen, Bo, Oddershede, Jette, & Poulsen, Henning F. A multiple length scale description of the mechanism of elastomer stretching. United States. https://doi.org/10.1039/c6ra22802j
Neuefeind, Joerg C., Skov, Anne L., Daniels, John E., Honkimaeki, Veijo, Jakobsen, Bo, Oddershede, Jette, and Poulsen, Henning F. Mon .
"A multiple length scale description of the mechanism of elastomer stretching". United States. https://doi.org/10.1039/c6ra22802j. https://www.osti.gov/servlets/purl/1328263.
@article{osti_1328263,
title = {A multiple length scale description of the mechanism of elastomer stretching},
author = {Neuefeind, Joerg C. and Skov, Anne L. and Daniels, John E. and Honkimaeki, Veijo and Jakobsen, Bo and Oddershede, Jette and Poulsen, Henning F.},
abstractNote = {Conventionally, the stretching of rubber is modeled exclusively by rotations of segments of the embedded polymer chains; i.e. changes in entropy. However models have not been tested on all relevant length scales due to a lack of appropriate probes. Here we present a universal X-ray based method for providing data on the structure of rubbers in the 2–50 Å range. First results relate to the elongation of a silicone rubber. We identify several non-entropic contributions to the free energy and describe the associated structural changes. By far the largest contribution comes from structural changes within the individual monomers, but among the contributions is also an elastic strain, acting between chains, which is 3–4 orders of magnitude smaller than the macroscopic strain, and of the opposite sign, i.e. extension of polymer chains in the direction perpendicular to the stretch. We find this may be due to trapped entanglements relaxing to positions close to the covalent crosslinks.},
doi = {10.1039/c6ra22802j},
journal = {RSC Advances},
number = 98,
volume = 6,
place = {United States},
year = {Mon Oct 03 00:00:00 EDT 2016},
month = {Mon Oct 03 00:00:00 EDT 2016}
}
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Works referenced in this record:
Spatial Configuration of Macromolecular Chains
journal, June 1975
- Flory, P. J.
- Science, Vol. 188, Issue 4195
Structure–mechanical property correlations of model siloxane elastomers with controlled network topology
journal, January 2009
- Urayama, Kenji; Kawamura, Takanobu; Kohjiya, Shinzo
- Polymer, Vol. 50, Issue 2
Thermal Fluctuations and Rubber Elasticity
journal, February 2007
- Xing, Xiangjun; Goldbart, Paul M.; Radzihovsky, Leo
- Physical Review Letters, Vol. 98, Issue 7
Tube Models for Rubber−Elastic Systems
journal, July 2001
- Mergell, Boris; Everaers, Ralf
- Macromolecules, Vol. 34, Issue 16
Dynamic mechanical response of polymer networks
journal, January 2000
- Edwards, S. F.; Takano, H.; Terentjev, E. M.
- The Journal of Chemical Physics, Vol. 113, Issue 13
Nonaffine Deformation and Elasticity of Polymer Networks
journal, December 1997
- Rubinstein, Michael; Panyukov, Sergei
- Macromolecules, Vol. 30, Issue 25
Test of the Foundations of Classical Rubber Elasticity
journal, October 1995
- Everaers, Ralf; Kremer, Kurt
- Macromolecules, Vol. 28, Issue 21
Giant fluctuations of crosslink positions in gels
journal, January 1992
- Rubinstein, Michael; Leibler, Ludwik; Bastide, Jacques
- Physical Review Letters, Vol. 68, Issue 3
Theory of long-range correlations in polymer melts
journal, January 1979
- de Gennes, P. G.
- Faraday Discussions of the Chemical Society, Vol. 68
The statistical mechanics of polymerized material
journal, September 1967
- Edwards, S. F.
- Proceedings of the Physical Society, Vol. 92, Issue 1
Soft Materials with Recoverable Shape Factors from Extreme Distortion States
journal, January 2016
- Goff, Jonathan; Sulaiman, Santy; Arkles, Barry
- Advanced Materials, Vol. 28, Issue 12
Elastic Properties of Nonstoichiometric Reacted PDMS Networks
journal, December 2003
- Larsen, A. L.; Hansen, K.; Sommer-Larsen, P.
- Macromolecules, Vol. 36, Issue 26
Small-Angle Neutron Scattering Investigation of Topological Constraints and Tube Deformation in Networks
journal, May 1995
- Straube, E.; Urban, V.; Pyckhout-Hintzen, W.
- Physical Review Letters, Vol. 74, Issue 22
Strain-Dependent Localization, Microscopic Deformations, and Macroscopic Normal Tensions in Model Polymer Networks
journal, December 2004
- Svaneborg, Carsten; Grest, Gary S.; Everaers, Ralf
- Physical Review Letters, Vol. 93, Issue 25
Local Order and Induced Orientation in PDMS Model Networks, Studied by 2 H NMR
journal, June 1998
- Sotta, P.
- Macromolecules, Vol. 31, Issue 12
Structure of Poly(dimethylsiloxane) Melts: Theory, Simulation, and Experiment
journal, July 2002
- Sides, Scott W.; Curro, John; Grest, Gary S.
- Macromolecules, Vol. 35, Issue 16
Amorphous silica studied by high energy X-ray diffraction
journal, July 1995
- Poulsen, H. F.; Neuefeind, J.; Neumann, H. -B.
- Journal of Non-Crystalline Solids, Vol. 188, Issue 1-2
Large amplitude oscillatory extension of soft polymeric networks
journal, June 2010
- Bejenariu, Anca Gabriela; Rasmussen, Henrik Koblitz; Skov, Anne Ladegaard
- Rheologica Acta, Vol. 49, Issue 8
Reversed planar elongation of soft polymeric networks
journal, June 2011
- Jensen, Mette Krog; Rasmussen, Henrik Koblitz; Skov, Anne Ladegaard
- Rheologica Acta, Vol. 50, Issue 9-10
Planar elongation of soft polymeric networks
journal, September 2009
- Jensen, Mette Krog; Hassager, Ole; Rasmussen, Henrik Koblitz
- Rheologica Acta, Vol. 49, Issue 1
Monochromators for High-Energy Synchrotron Radiation
journal, January 2001
- Suortti, P.; Buslaps, T.; Honkimäki, V.
- Zeitschrift für Physikalische Chemie, Vol. 215, Issue 11
High-energy X-ray diffraction using the Pixium 4700 flat-panel detector
journal, May 2009
- Daniels, J. E.; Drakopoulos, M.
- Journal of Synchrotron Radiation, Vol. 16, Issue 4
The diffraction of X-rays by a random assemblage of molecules having partial alignment
journal, July 1952
- Deas, H. D.
- Acta Crystallographica, Vol. 5, Issue 4
Application of cylindrical distribution functions to wide-angle X-ray scattering from oriented polymers
journal, March 1981
- Mitchell, G. R.; Lovell, R.
- Acta Crystallographica Section A, Vol. 37, Issue 2
Crystallinity and orientation in silicone rubber. I. X-ray studies
journal, January 1958
- Ohlberg, Stanley M.; Alexander, Leroy E.; Warrick, E. L.
- Journal of Polymer Science, Vol. 27, Issue 115
Measuring strain distributions in amorphous materials
journal, December 2004
- Poulsen, Henning F.; Wert, John A.; Neuefeind, Jörg
- Nature Materials, Vol. 4, Issue 1
Connection between Polymer Molecular Weight, Density, Chain Dimensions, and Melt Viscoelastic Properties
journal, August 1994
- Fetters, L. J.; Lohse, D. J.; Richter, D.
- Macromolecules, Vol. 27, Issue 17
Improved United Atom Force Field for Poly(dimethylsiloxane)
journal, March 2003
- Frischknecht, Amalie L.; Curro, John G.
- Macromolecules, Vol. 36, Issue 6
Elastic Properties of Polymer Networks
journal, September 1996
- Everaers, Ralf; Kremer, Kurt
- Journal of Molecular Modeling, Vol. 2, Issue 9
Beziehungen zwischen elastischen Konstanten und Dehnungsdoppelbrechung hochelastischer Stoffe
journal, December 1942
- Kuhn, Werner; Grün, F.
- Kolloid-Zeitschrift, Vol. 101, Issue 3
Electromechanical stability of compressible dielectric elastomer actuators
journal, October 2011
- Liu, Liwu; Liu, Yanju; Leng, Jinsong
- Smart Materials and Structures, Vol. 20, Issue 11
Thermo-electro-mechanical instability of dielectric elastomers
journal, May 2011
- Liu, Liwu; Liu, Yanju; Li, Bo
- Smart Materials and Structures, Vol. 20, Issue 7
Theory of dielectric elastomers
journal, December 2010
- Suo, Zhigang
- Acta Mechanica Solida Sinica, Vol. 23, Issue 6
Theory of Dielectric Elastomers Capable of Giant Deformation of Actuation
journal, April 2010
- Zhao, Xuanhe; Suo, Zhigang
- Physical Review Letters, Vol. 104, Issue 17
The Current State of Silicone-Based Dielectric Elastomer Transducers
journal, January 2016
- Madsen, Frederikke B.; Daugaard, Anders E.; Hvilsted, Søren
- Macromolecular Rapid Communications, Vol. 37, Issue 5
Works referencing / citing this record:
Optimization Techniques for Improving the Performance of Silicone-Based Dielectric Elastomers
journal, November 2017
- Skov, Anne Ladegaard; Yu, Liyun
- Advanced Engineering Materials, Vol. 20, Issue 5
Molecular Strategies for Improved Dielectric Elastomer Electrical Breakdown Strengths
journal, July 2018
- Yu, Liyun; Skov, Anne L.
- Macromolecular Rapid Communications, Vol. 39, Issue 16
Anisotropic and heterogeneous dynamics in stretched elastomer nanocomposites
journal, January 2019
- Ehrburger-Dolle, Françoise; Morfin, Isabelle; Bley, Françoise
- Soft Matter, Vol. 15, Issue 18