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Title: Gamma Irradiation and Oxidative Degradation of a Silica-Filled Silicone Elastomer

Abstract

The radiation oxidative degradation of a commonly used silica-filled silicone elastomer DC745 was investigated by a series of experimental techniques. This elastomer is known to be chemically and thermally stable, but insufficient data exist on the radiation resistance. In the present work, gamma doses up to 200 kGy were applied under air at RT and 1Gy/s. Radiation chemical changes were investigated by NMR, FT-IR, Raman, and mass spectroscopy. DSC and TGA experiments probed thermal transitions and thermal stability changes with exposure dose. SEM probed variations on the surface of the elastomer, and solvent swelling methods were used to investigate changes in the polymer network properties. Electron paramagnetic resonance was employed to detect and identify free radicals. Uniaxial compression load tests at variable temperatures were performed to assess changes in the material’s mechanical response as a function of radiation dose. Results demonstrate that, with increasing exposure, DC745 undergoes changes in chemistry that lead to an increase in thermal stability and cross-link density, formation of free radical species, decrease in heat of fusion and increase in stiffness at low temperatures. Taken together, these results indicate that oxidative cross-linking is the dominant radiolysis mechanism that occurs when this material is exposed to gammamore » irradiation in air at high dose rates.« less

Authors:
 [1];  [2];  [1];  [2];  [1];  [2];  [2];  [3];  [3]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Chemical Diagnostic and Engineering
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Division of Materials Science and Technology
  3. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Materials Characterization and Performance Dept.
Publication Date:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1329567
Alternate Identifier(s):
OSTI ID: 1245280
Report Number(s):
LA-UR-15-21100
Journal ID: ISSN 0141-3910
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Polymer Degradation and Stability
Additional Journal Information:
Journal Volume: 116; Journal ID: ISSN 0141-3910
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; PDMS, irradiation; oxidative degradation; radiolysis

Citation Formats

Labouriau, Andrea, Cady, Carl Mcelhinney, Gill, John T., Stull, Jamie Ann, Ortiz-Acosta, Denisse, Henderson, Kevin C., Hartung, Vaughn, Quintana, Adam, and Celina, Mathew C. Gamma Irradiation and Oxidative Degradation of a Silica-Filled Silicone Elastomer. United States: N. p., 2015. Web. doi:10.1016/j.polymdegradstab.2015.03.009.
Labouriau, Andrea, Cady, Carl Mcelhinney, Gill, John T., Stull, Jamie Ann, Ortiz-Acosta, Denisse, Henderson, Kevin C., Hartung, Vaughn, Quintana, Adam, & Celina, Mathew C. Gamma Irradiation and Oxidative Degradation of a Silica-Filled Silicone Elastomer. United States. https://doi.org/10.1016/j.polymdegradstab.2015.03.009
Labouriau, Andrea, Cady, Carl Mcelhinney, Gill, John T., Stull, Jamie Ann, Ortiz-Acosta, Denisse, Henderson, Kevin C., Hartung, Vaughn, Quintana, Adam, and Celina, Mathew C. Sat . "Gamma Irradiation and Oxidative Degradation of a Silica-Filled Silicone Elastomer". United States. https://doi.org/10.1016/j.polymdegradstab.2015.03.009. https://www.osti.gov/servlets/purl/1329567.
@article{osti_1329567,
title = {Gamma Irradiation and Oxidative Degradation of a Silica-Filled Silicone Elastomer},
author = {Labouriau, Andrea and Cady, Carl Mcelhinney and Gill, John T. and Stull, Jamie Ann and Ortiz-Acosta, Denisse and Henderson, Kevin C. and Hartung, Vaughn and Quintana, Adam and Celina, Mathew C.},
abstractNote = {The radiation oxidative degradation of a commonly used silica-filled silicone elastomer DC745 was investigated by a series of experimental techniques. This elastomer is known to be chemically and thermally stable, but insufficient data exist on the radiation resistance. In the present work, gamma doses up to 200 kGy were applied under air at RT and 1Gy/s. Radiation chemical changes were investigated by NMR, FT-IR, Raman, and mass spectroscopy. DSC and TGA experiments probed thermal transitions and thermal stability changes with exposure dose. SEM probed variations on the surface of the elastomer, and solvent swelling methods were used to investigate changes in the polymer network properties. Electron paramagnetic resonance was employed to detect and identify free radicals. Uniaxial compression load tests at variable temperatures were performed to assess changes in the material’s mechanical response as a function of radiation dose. Results demonstrate that, with increasing exposure, DC745 undergoes changes in chemistry that lead to an increase in thermal stability and cross-link density, formation of free radical species, decrease in heat of fusion and increase in stiffness at low temperatures. Taken together, these results indicate that oxidative cross-linking is the dominant radiolysis mechanism that occurs when this material is exposed to gamma irradiation in air at high dose rates.},
doi = {10.1016/j.polymdegradstab.2015.03.009},
journal = {Polymer Degradation and Stability},
number = ,
volume = 116,
place = {United States},
year = {Sat Mar 21 00:00:00 EDT 2015},
month = {Sat Mar 21 00:00:00 EDT 2015}
}

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Cited by: 32 works
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Works referenced in this record:

The radiation chemistry of some polysiloxanes: An electron spin resonance study
journal, January 1963


Radiation-Induced Cross-Linking in a Silica-Filled Silicone Elastomer As Investigated by Multiple Quantum 1 H NMR
journal, August 2005

  • Maxwell, Robert S.; Chinn, Sarah C.; Solyom, David
  • Macromolecules, Vol. 38, Issue 16
  • DOI: 10.1021/ma047625s

Qualification of automated low-field NMR relaxometry for quality control of polymers in a production setting
journal, December 2007


Modelling molecular weight changes induced in polydimethylsiloxane by gamma and electron beam irradiation
journal, May 2008


Polydimethylsiloxane thermal degradation Part 1. Kinetic aspects
journal, March 2001


A quick, direct method for the determination of activation energy from thermogravimetric data
journal, May 1966

  • Flynn, Joseph H.; Wall, Leo A.
  • Journal of Polymer Science Part B: Polymer Letters, Vol. 4, Issue 5
  • DOI: 10.1002/pol.1966.110040504

General and efficient simulation of pulse EPR spectra
journal, January 2009

  • Stoll, Stefan; Britt, R. David
  • Physical Chemistry Chemical Physics, Vol. 11, Issue 31
  • DOI: 10.1039/b907277b

EasySpin, a comprehensive software package for spectral simulation and analysis in EPR
journal, January 2006


NH3-modified swelling of silica-filled silicone rubber
journal, May 1979


Interaction of polydimethylsiloxanes with swelling agents
journal, January 1955


Oxygen Permeability Measurements on Elastomers at Temperatures up to 225 °C
journal, April 2005


Review of polymer oxidation and its relationship with materials performance and lifetime prediction
journal, December 2013


Time development of diffusion-limited oxidation profiles in a radiation environment
journal, May 1997


Rigorous experimental confirmation of a theoretical model for diffusion-limited oxidation
journal, January 1992


An ultrasensitive technique for testing the Arrhenius extrapolation assumption for thermally aged elastomers
journal, January 1995


A perspective on the inherent oxidation sensitivity of epoxy materials
journal, June 2013


Structure-permeability relationships in silicone polymers
journal, June 1987

  • Stern, S. A.; Shah, V. M.; Hardy, B. J.
  • Journal of Polymer Science Part B: Polymer Physics, Vol. 25, Issue 6
  • DOI: 10.1002/polb.1987.090250607

High-energy radiation and polymers: A review of commercial processes and emerging applications
journal, December 2001

  • Clough, R. L.
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 185, Issue 1-4
  • DOI: 10.1016/S0168-583X(01)00966-1

Crystallization of polydimethylsiloxane end-linked networks
journal, December 2000


Nuclear magnetic resonance and principal component analysis for investigating the degradation of poly[chlorotrifluoroethylene-co-(vinylidene fluoride)] by ionizing radiation
journal, July 2012


The radiation chemistry of poly(dimethyl-siloxane)
journal, July 2000


A signal-to-noise standard for pulsed EPR
journal, July 2010

  • Eaton, Gareth R.; Eaton, Sandra S.; Quine, Richard W.
  • Journal of Magnetic Resonance, Vol. 205, Issue 1
  • DOI: 10.1016/j.jmr.2010.04.006

Linear transformation of EPR spectra as a method proposed for improving identification of paramagnetic species in ceramic
journal, April 2007


Characteristic of paramagnetic centres in burnt clay and pottery by the EPR method
journal, February 2007


Theoretical modeling of the Al paramagnetic center and its precursors in stishovite
journal, June 2009


The structure of the colour centres in smoky quartz
journal, September 1955

  • O'Brien, Mary C. M.
  • Proceedings of the Royal Society of London. Series A. Mathematical and Physical Sciences, Vol. 231, Issue 1186, p. 404-414
  • DOI: 10.1098/rspa.1955.0183

Oxygen-excess-related point defects in glassy/amorphous SiO2 and related materials
journal, September 2012

  • Skuja, L.; Kajihara, K.; Hirano, M.
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 286
  • DOI: 10.1016/j.nimb.2012.02.038

Effects of iron on the formation and annihilation of X-ray irradiation induced non-bridging oxygen hole centers in soda-lime silicate glass
journal, February 2010


Electron spin resonance measurement of radiation-induced defects and reactions in vitreous silica irradiated with ion beams
journal, February 2008


An e.s.r. study of the motion of peroxy radicals in isotactic and atactic polypropylenes
journal, October 1984


A review on the Mullins effect
journal, March 2009


Works referencing / citing this record:

Dielectric and Carrier Transport Properties of Silicone Rubber Degraded by Gamma Irradiation
journal, October 2017


Experimental investigation of the degradation mechanism of silicone rubber exposed to heat and gamma rays
journal, June 2017


Inorganic fillers influence on the radiation-induced ageing of a space-used silicone elastomer
journal, June 2016