Constitutive Model of Radiation Aging Effects in Filled Silicone Elastomers under Strain

Maiti, A.; Small, W.; Kroonblawd, M. P.; Lewicki, J. P.; Goldman, N.; Wilson, T. S.; Saab, A. P.

doi:10.1021/acs.jpcb.1c04958

Title: Constitutive Model of Radiation Aging Effects in Filled Silicone Elastomers under Strain

Journal Article · Fri Aug 27 00:00:00 EDT 2021 · Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry

DOI:https://doi.org/10.1021/acs.jpcb.1c04958· OSTI ID:1826874

^[1]; Small, W. ^[1];

^[1];

^[1]; Wilson, T. S. ^[1]; Saab, A. P. ^[1]

Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

Filled silicone elastomers, an essential component in many technological applications, are often subjected to controlled or unintended radiation for a variety of reasons. Radiation exposure can lead to permanent mechanical and structural changes in the material, which is manifested as altered mechanical response, and in some cases, a permanent set. For unfilled elastomers, network theories developed and refined over decades can explain these effects in terms of chain-scission and cross-link formation and a hypothesis involving independent networks formed at different strain levels of the material. In this work, we expose a filled silicone rubber to gamma radiation while being under finite elongational strain and show that the observed mechanical and structural changes can be quantitatively modeled within the same theoretical framework developed for unfilled elastomers as long as nuances associated with the Mullins effect are accounted for in a consistent manner. In this work, we employ Ogden’s incompressible hyperelastic model within the framework of Tobolsky’s two-network scheme to describe the observed permanent set and mechanical modulus changes as a function of radiation dosage. In the process, we conclude that gamma radiation induces both direct cross-linking at chain crossings (H-links) and main-chain-scission followed by cross-linking (Y-links). We provide an estimate of the ratio of chain-scission to cross-linking rates, which is in reasonable agreement with previous experimental estimate from Charlesby–Pinner analysis. We use density functional theory (DFT)-based quantum mechanical calculations to explore the stability of –Si and –SiO radicals that form upon a radiation-induced chain-scission event, which sheds light on the relative rates of Y-linking and H-linking processes.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1826874

Report Number(s):: LLNL-JRNL-822068; 1033964

Journal Information:: Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry, Vol. 125, Issue 35; ISSN 1520-6106

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (54)

Large Deformation Isotropic Elasticity - On the Correlation of Theory and Experiment for Incompressible Rubberlike Solids Ogden, R. W. Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 326, Issue 1567 https://doi.org/10.1098/rspa.1972.0026	journal	February 1972
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Reaction Mechanisms in Irradiated, Precipitated, and Mesoporous Silica Dondi, D.; Buttafava, A.; Zeffiro, A. The Journal of Physical Chemistry A, Vol. 117, Issue 16 https://doi.org/10.1021/jp310683e	journal	April 2013
Elasticity of Polymer Networks Rubinstein, Michael; Panyukov, Sergei Macromolecules, Vol. 35, Issue 17 https://doi.org/10.1021/ma0203849	journal	August 2002
On a molecular statistical basis for Ogden's model of rubber elasticity Ehret, Alexander E. Journal of the Mechanics and Physics of Solids, Vol. 78 https://doi.org/10.1016/j.jmps.2015.02.006	journal	May 2015
Two-scale mechanism-based theory of nonlinear viscoelasticity Tang, Shan; Steven Greene, M.; Liu, Wing Kam Journal of the Mechanics and Physics of Solids, Vol. 60, Issue 2 https://doi.org/10.1016/j.jmps.2011.11.003	journal	February 2012
Coupling effects of gamma irradiation and absorbed moisture on silicone foam Wang, Pu-Cheng; Yang, Na; Liu, Dong Materials & Design, Vol. 195 https://doi.org/10.1016/j.matdes.2020.108998	journal	October 2020
Kinetics of decay of methyl radicals in irradiated dimethylsilanediol and polymethylsiloxanes Pankratova, Lidiya N.; Saenko, Elizaveta V.; Bugaenko, Vladislav L. Mendeleev Communications, Vol. 21, Issue 3 https://doi.org/10.1016/j.mencom.2011.04.016	journal	May 2011
Thermal stability and corrosion resistance of polysiloxane coatings on 2024-T3 and 6061-T6 aluminum alloy Wu, K. H.; Chao, C. M.; Yeh, T. F. Surface and Coatings Technology, Vol. 201, Issue 12 https://doi.org/10.1016/j.surfcoat.2006.10.024	journal	March 2007
An investigation of the theory of rubber elasticity using irradiated polydimethylsiloxanes Bueche, A. M. Journal of Polymer Science, Vol. 19, Issue 92 https://doi.org/10.1002/pol.1956.120199206	journal	February 1956
A nonaffine network model for elastomers undergoing finite deformations Davidson, Jacob D.; Goulbourne, N. C. Journal of the Mechanics and Physics of Solids, Vol. 61, Issue 8 https://doi.org/10.1016/j.jmps.2013.03.009	journal	August 2013
Comparison of Hyperelastic Models for Rubber-Like Materials Marckmann, G.; Verron, E. Rubber Chemistry and Technology, Vol. 79, Issue 5 https://doi.org/10.5254/1.3547969	journal	November 2006
Effect of Strain History on Stress and Permanent Set in Cross-Linking Networks: A Molecular Dynamics Study Rottach, Dana R.; Curro, John G.; Grest, Gary S. Macromolecules, Vol. 37, Issue 14 https://doi.org/10.1021/ma049723j	journal	July 2004
Effect of Stretching on the Properties of Rubber Mullins, L. Rubber Chemistry and Technology, Vol. 21, Issue 2 https://doi.org/10.5254/1.3546914	journal	June 1948
Molecular Dynamics Simulations of Polymer Networks Undergoing Sequential Cross-Linking and Scission Reactions Rottach, Dana R.; Curro, John G.; Budzien, Joanne Macromolecules, Vol. 40, Issue 1 https://doi.org/10.1021/ma062139l	journal	January 2007
Radiation-induced mechanical property changes in filled rubber Maiti, A.; Weisgraber, T. H.; Gee, R. H. Physical Review E, Vol. 83, Issue 6 https://doi.org/10.1103/PhysRevE.83.062801	journal	June 2011
Complexities associated with moisture in foamed polysiloxane composites Patel, Mogon; Morrell, Paul; Cunningham, Jenny Polymer Degradation and Stability, Vol. 93, Issue 2 https://doi.org/10.1016/j.polymdegradstab.2007.10.026	journal	February 2008
Tube theory of entangled polymer dynamics McLeish, T. C. B. Advances in Physics, Vol. 51, Issue 6 https://doi.org/10.1080/00018730210153216	journal	September 2002
Gamma Irradiation of Silicones Palsule, Aniruddha S.; Clarson, Stephen J.; Widenhouse, Christopher W. Journal of Inorganic and Organometallic Polymers and Materials, Vol. 18, Issue 2 https://doi.org/10.1007/s10904-008-9205-0	journal	April 2008
Molecular weight changes and scission and crosslinking in poly(dimethyl siloxane) on gamma radiolysis Hill, David J. T.; Preston, Christopher M. L.; Salisbury, Daniel J. Radiation Physics and Chemistry, Vol. 62, Issue 1 https://doi.org/10.1016/S0969-806X(01)00416-9	journal	July 2001
Effect of Polymer-Filler and Filler-Filler Interactions on Dynamic Properties of Filled Vulcanizates Wang, Meng-Jiao Rubber Chemistry and Technology, Vol. 71, Issue 3 https://doi.org/10.5254/1.3538492	journal	July 1998
A Full-Network Rubber Elasticity Model based on Analytical Integration Itskov, Mikhail; Ehret, Alexander E.; Dargazany, Roozbeh Mathematics and Mechanics of Solids, Vol. 15, Issue 6 https://doi.org/10.1177/1081286509106441	journal	June 2009
The effect of entanglements in rubber elasticity Edwards, S. F.; Vilgis, Th. Polymer, Vol. 27, Issue 4 https://doi.org/10.1016/0032-3861(86)90231-4	journal	April 1986
Theoretical Model of Polymer Network Chain Formation under Strain Yu, Yong; Yan, Shunping; Fang, Ye ACS Omega, Vol. 3, Issue 11 https://doi.org/10.1021/acsomega.8b01748	journal	November 2018
A reciprocal space based method for treating long range interactions in ab initio and force-field-based calculations in clusters Martyna, Glenn J.; Tuckerman, Mark E. The Journal of Chemical Physics, Vol. 110, Issue 6 https://doi.org/10.1063/1.477923	journal	February 1999
A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu Grimme, Stefan; Antony, Jens; Ehrlich, Stephan The Journal of Chemical Physics, Vol. 132, Issue 15 https://doi.org/10.1063/1.3382344	journal	April 2010
Anisotropic Hydrolysis Susceptibility in Deformed Polydimethylsiloxanes Kroonblawd, Matthew P.; Goldman, Nir; Lewicki, James P. The Journal of Physical Chemistry B, Vol. 123, Issue 37 https://doi.org/10.1021/acs.jpcb.9b07159	journal	August 2019
Self-Consistent Equations Including Exchange and Correlation Effects Kohn, W.; Sham, L. J. Physical Review, Vol. 140, Issue 4A, p. A1133-A1138 https://doi.org/10.1103/PhysRev.140.A1133	journal	November 1965
Chemical Degradation Pathways in Siloxane Polymers Following Phenyl Excitations Kroonblawd, Matthew P.; Goldman, Nir; Lewicki, James P. The Journal of Physical Chemistry B, Vol. 122, Issue 50 https://doi.org/10.1021/acs.jpcb.8b09636	journal	November 2018
Permanent Set of Cross-Linking Networks: Comparison of Theory with Molecular Dynamics Simulations Rottach, Dana R.; Curro, John G.; Budzien, Joanne Macromolecules, Vol. 39, Issue 16 https://doi.org/10.1021/ma060767x	journal	August 2006
A three-dimensional constitutive model for the large stretch behavior of rubber elastic materials Arruda, Ellen M.; Boyce, Mary C. Journal of the Mechanics and Physics of Solids, Vol. 41, Issue 2 https://doi.org/10.1016/0022-5096(93)90013-6	journal	February 1993
CP2K: An electronic structure and molecular dynamics software package - Quickstep: Efficient and accurate electronic structure calculations Kühne, Thomas D.; Iannuzzi, Marcella; Del Ben, Mauro The Journal of Chemical Physics, Vol. 152, Issue 19 https://doi.org/10.1063/5.0007045	journal	May 2020
Radiation Chemistry of Polydimethylsiloxane. ¹ I. Crosslinking and Gas Yields Miller, A. A. Journal of the American Chemical Society, Vol. 82, Issue 14 https://doi.org/10.1021/ja01499a011	journal	July 1960
Properties and Structure of Polymers Tobolsky, Arthur V.; Callinan, Thomas D. Journal of The Electrochemical Society, Vol. 107, Issue 10 https://doi.org/10.1149/1.2427514	journal	January 1960
Radiation Chemistry of Polydimethylsiloxane. ¹ II. Effects of Additives Miller, A. A. Journal of the American Chemical Society, Vol. 83, Issue 1 https://doi.org/10.1021/ja01462a006	journal	January 1961
Elasticity of polymer networks cross-linked in states of strain Flory, P. J. Transactions of the Faraday Society, Vol. 56 https://doi.org/10.1039/tf9605600722	journal	January 1960
The radiation chemistry of some polysiloxanes: An electron spin resonance study Ormerod, M. G.; Charlesby, A. Polymer, Vol. 4 https://doi.org/10.1016/0032-3861(63)90059-4	journal	January 1963
Softening of Rubber by Deformation Mullins, L. Rubber Chemistry and Technology, Vol. 42, Issue 1 https://doi.org/10.5254/1.3539210	journal	March 1969
Constitutive modeling of the large strain time-dependent behavior of elastomers Bergstrom, J. Journal of the Mechanics and Physics of Solids, Vol. 46, Issue 5 https://doi.org/10.1016/S0022-5096(97)00075-6	journal	May 1998
Changes in silicone polymeric fluids due to high-energy radiation Charlesby, A. Proceedings of the Royal Society of London. Series A. Mathematical and Physical Sciences, Vol. 230, Issue 1180, p. 120-135 https://doi.org/10.1098/rspa.1955.0116	journal	June 1955
NMR study of the gamma radiolysis of poly(dimethyl siloxane) under vacuum at 303 K Hill, David J. T.; Preston, Christopher M. L.; Whittaker, Andrew K. Polymer, Vol. 43, Issue 4 https://doi.org/10.1016/S0032-3861(01)00711-X	journal	February 2002
Inhomogeneous Electron Gas Hohenberg, P.; Kohn, W. Physical Review, Vol. 136, Issue 3B, p. B864-B871 https://doi.org/10.1103/PhysRev.136.B864	journal	November 1964
A Quantum-Based Approach to Predict Primary Radiation Damage in Polymeric Networks Kroonblawd, Matthew P.; Goldman, Nir; Maiti, Amitesh Journal of Chemical Theory and Computation, Vol. 17, Issue 1 https://doi.org/10.1021/acs.jctc.0c00967	journal	December 2020
Quantification of radiation induced crosslinking in a commercial, toughened silicone rubber, TR55 by 1H MQ-NMR Maxwell, Robert S.; Chinn, Sarah C.; Alviso, Cynthia T. Polymer Degradation and Stability, Vol. 94, Issue 3 https://doi.org/10.1016/j.polymdegradstab.2008.10.028	journal	March 2009
RADIATION CHEMISTRY OF HEXAMETHYLDISILOXANE, A POLYDIMETHYLSILOXANE MODEL ¹ Dewhurst, H. A.; Pierre, L. E. St. The Journal of Physical Chemistry, Vol. 64, Issue 8 https://doi.org/10.1021/j100837a025	journal	August 1960
Bulk and surface modification of silicone rubber for biomedical applications Abbasi, Farhang; Mirzadeh, Hamid; Katbab, Ali-Asgar Polymer International, Vol. 51, Issue 10 https://doi.org/10.1002/pi.1069	journal	January 2002
The role of silica in radiation induced grafting and crosslinking of silica/elastomers blends Dondi, D.; Buttafava, A.; Zeffiro, A. Polymer, Vol. 53, Issue 21 https://doi.org/10.1016/j.polymer.2012.08.015	journal	September 2012
Silicone elastomers for electronic applications. I. Analyses of the noncrosslinked fractions Andersson, L. H. U.; Hjertberg, T. Journal of Applied Polymer Science, Vol. 88, Issue 8 https://doi.org/10.1002/app.12027	journal	March 2003
A review on the Mullins effect Diani, Julie; Fayolle, Bruno; Gilormini, Pierre European Polymer Journal, Vol. 45, Issue 3 https://doi.org/10.1016/j.eurpolymj.2008.11.017	journal	March 2009
Reptation of a Polymer Chain in the Presence of Fixed Obstacles de Gennes, P. G. The Journal of Chemical Physics, Vol. 55, Issue 2 https://doi.org/10.1063/1.1675789	journal	July 1971
Adhesion enhancement by a dielectric barrier discharge of PDMS used for flexible and stretchable electronics Morent, R.; De Geyter, N.; Axisa, F. Journal of Physics D: Applied Physics, Vol. 40, Issue 23, p. 7392-7401 https://doi.org/10.1088/0022-3727/40/23/021	journal	November 2007
Silicone sealants and structural adhesives de Buyl, François International Journal of Adhesion and Adhesives, Vol. 21, Issue 5 https://doi.org/10.1016/S0143-7496(01)00018-5	journal	January 2001
Surface modification of polymers for medical applications Ikada, Y. Biomaterials, Vol. 15, Issue 10 https://doi.org/10.1016/0142-9612(94)90025-6	journal	August 1994
Mullins effect in a filled elastomer under uniaxial tension Maiti, A.; Small, W.; Gee, R. H. Physical Review E, Vol. 89, Issue 1 https://doi.org/10.1103/PhysRevE.89.012602	journal	January 2014

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