Accelerated oxidation of epoxy thermosets with increased O2 pressure

Celina, Mathew C.; Linde, Carl Erik; Barrett, Matija Viola; Ko, Lisa Rose

doi:10.1016/j.polymdegradstab.2024.110886

Accelerated oxidation of epoxy thermosets with increased O₂ pressure

Journal Article · Wed Jun 19 00:00:00 EDT 2024 · Polymer Degradation and Stability

DOI:https://doi.org/10.1016/j.polymdegradstab.2024.110886· OSTI ID:2429941

^[1]; Linde, Carl Erik ^[1]; Barrett, Matija Viola ^[1]; Ko, Lisa Rose ^[1]

Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Polymer oxidation is usually accelerated with temperature, which is therefore applied in nearly every experimental approach dealing with predictive materials aging. Because of this simple approach, we may tend to neglect that the effective concentration of oxygen also acts as a rate multiplier for oxidation. Increasing the oxygen partial pressure in an aging environment accelerates oxidation, and while there is often a near proportional increase initially, the effect of additional oxygen usually transitions to a saturation level at some elevated pressure. This has been theoretically described in the general autoxidation scheme and is well recognized. However, for many materials the exact rate behavior under moderately increased oxygen concentration remains to be established. We therefore review epoxy oxidation and offer a broader overview of its behavior under increased O₂ partial pressure. Experimental data are given for a few thermoset materials demonstrating their rate behavior under O₂ partial pressure up to 4 atm, meaning approximately 20 times more than under standard atmospheric conditions. Confirmative evidence suggests that epoxy materials will reach saturation oxidation rates only at significantly higher O₂ partial pressure. In such a high-pressure regime it is theoretically possible to not only accelerate oxidation, but to transition into a condition where O₂ diffusion can be increased without further accelerating the oxidation rate. Finally, this can reduce diffusion limited oxidation effects under specific accelerated aging conditions as a combination of temperature and O₂ partial pressure.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: NA0003525

OSTI ID:: 2429941

Report Number(s):: SAND--2024-10556J

Journal Information:: Polymer Degradation and Stability, Journal Name: Polymer Degradation and Stability Journal Issue: 1 Vol. 228; ISSN 0141-3910

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (59)

Accelerated thermal aging of NBR and other materials under air or oxygen pressures Budrugeac, Petru Die Angewandte Makromolekulare Chemie, Vol. 247, Issue 1 https://doi.org/10.1002/apmc.1997.052470102	journal	May 1997
Gas transport in halogen‐containing aromatic polycarbonates Hellums, M. W.; Koros, W. J.; Husk, G. R. Journal of Applied Polymer Science, Vol. 43, Issue 11 https://doi.org/10.1002/app.1991.070431103	journal	December 1991
Lifetime prediction of polymers Hamid, S. H.; Amin, M. B. Journal of Applied Polymer Science, Vol. 55, Issue 10 https://doi.org/10.1002/app.1995.070551003	journal	March 1995
Thermal oxidation kinetics for a poly(bismaleimide) Colin, X.; Marais, C.; Verdu, J. Journal of Applied Polymer Science, Vol. 82, Issue 14 https://doi.org/10.1002/app.2203	journal	October 2001
Autoxidation of poly-4-methylpentene-1. I. The role of diffusion in autoxidation kinetics Billingham, N. C.; Walker, T. J. Journal of Polymer Science: Polymer Chemistry Edition, Vol. 13, Issue 5 https://doi.org/10.1002/pol.1975.170130515	journal	May 1975
“Close loop” mechanistic schemes for hydrocarbon polymer oxidation Audouin, L.; Gueguen, V.; Tcharkhtchi, A. Journal of Polymer Science Part A: Polymer Chemistry, Vol. 33, Issue 6 https://doi.org/10.1002/pola.1995.080330605	journal	April 1995
Role of oxygen diffusion in polymer ageing: kinetic and mechanical aspects Audouin, L.; Langlois, V.; Verdu, J. Journal of Materials Science, Vol. 29, Issue 3 https://doi.org/10.1007/BF00445968	journal	February 1994
Prediction of service lifetimes of elastomeric seals during radiation ageing Burnay, S. G.; Hitchon, J. W. Journal of Nuclear Materials, Vol. 131, Issue 2-3 https://doi.org/10.1016/0022-3115(85)90458-1	journal	April 1985
Rigorous experimental confirmation of a theoretical model for diffusion-limited oxidation Gillen, Kenneth T.; Clough, Roger L. Polymer, Vol. 33, Issue 20 https://doi.org/10.1016/0032-3861(92)90280-A	journal	January 1992
Initiated oxidation of polypropylene, polypropylene-polyethylene mixtures, and ethylene-propylene copolymers Shilov, Yu. B.; Denisov, Ye. T. Polymer Science U.S.S.R., Vol. 14, Issue 11 https://doi.org/10.1016/0032-3950(72)90207-9	journal	January 1972
The diffusional regime in the initiated oxidation of polymers Denisov, Ye. T.; Shilov, Yu. B. Polymer Science U.S.S.R., Vol. 25, Issue 6 https://doi.org/10.1016/0032-3950(83)90074-6	journal	January 1983
A model for diffusion in a glassy polymer Vieth, W. R.; Sladek, K. J. Journal of Colloid Science, Vol. 20, Issue 9 https://doi.org/10.1016/0095-8522(65)90071-1	journal	December 1965
Photo-oxidation of thick polymer samples—Part II: The influence of oxygen diffusion on the natural and artificial weathering of polyolefins Cunliffe, A. V.; Davis, A. Polymer Degradation and Stability, Vol. 4, Issue 1 https://doi.org/10.1016/0141-3910(82)90003-9	journal	January 1982
Modulus profiling of polymers Gillen, Kenneth T.; Clough, Roger L.; Quintana, Carlos A. Polymer Degradation and Stability, Vol. 17, Issue 1 https://doi.org/10.1016/0141-3910(87)90046-2	journal	January 1987
Oxygen diffusion effects in thermally aged elastomers Clough, R. L.; Gillen, K. T. Polymer Degradation and Stability, Vol. 38, Issue 1 https://doi.org/10.1016/0141-3910(92)90022-W	journal	January 1992
An ultrasensitive technique for testing the Arrhenius extrapolation assumption for thermally aged elastomers Wise, J.; Gillen, K. T.; Clough, R. L. Polymer Degradation and Stability, Vol. 49, Issue 3 https://doi.org/10.1016/0141-3910(95)00137-B	journal	January 1995
A review of oxygen uptake techniques for measuring polyolefin oxidation Scheirs, John; Bigger, Stephen W.; Billingham, Norman C. Polymer Testing, Vol. 14, Issue 3 https://doi.org/10.1016/0142-9418(94)00022-7	journal	January 1995
Anomalous aging phenomena in a crosslinked polyolefin cable insulation Celina, M.; Gillen, K. T.; Wise, J. Radiation Physics and Chemistry, Vol. 48, Issue 5 https://doi.org/10.1016/0969-806X(96)00083-7	journal	November 1996
Quantitative model for the time development of diffusion-limited oxidation profiles Wise, J.; Gillen, K. T.; Clough, R. L. Polymer, Vol. 38, Issue 8 https://doi.org/10.1016/S0032-3861(96)00716-1	journal	April 1997
Oxidation induced embrittlement in polypropylene — a tensile testing study Fayolle, B.; Audouin, L.; Verdu, J. Polymer Degradation and Stability, Vol. 70, Issue 3 https://doi.org/10.1016/S0141-3910(00)00108-7	journal	January 2000
A general solution of the closed-loop kinetic scheme for the thermal oxidation of polypropylene Rincon-Rubio, L. M.; Fayolle, B.; Audouin, L. Polymer Degradation and Stability, Vol. 74, Issue 1 https://doi.org/10.1016/S0141-3910(01)00154-9	journal	January 2001
Oxidation induced shrinkage for thermally aged epoxy networks Decelle, J.; Huet, N.; Bellenger, V. Polymer Degradation and Stability, Vol. 81, Issue 2 https://doi.org/10.1016/S0141-3910(03)00094-6	journal	January 2003
Chemical and morphological changes of environmentally degradable polyethylene films exposed to thermo-oxidation Khabbaz, Farideh; Albertsson, Ann-Christine; Karlsson, Sigbritt Polymer Degradation and Stability, Vol. 63, Issue 1 https://doi.org/10.1016/S0141-3910(98)00082-2	journal	January 1999
Preliminary evaluation of the use of elevated pressure to accelerate thermo-oxidative aging in composites Tsotsis, Thomas K.; Keller, Scott; Bardis, Jason Polymer Degradation and Stability, Vol. 64, Issue 2 https://doi.org/10.1016/S0141-3910(98)00190-6	journal	May 1999
A new method for predicting the thermal oxidation of thermoset matrices Colin, X.; Marais, C.; Verdu, J. Polymer Testing, Vol. 20, Issue 7 https://doi.org/10.1016/S0142-9418(01)00021-6	journal	January 2001
Aging of polymeric composite specimens for 5000 hours at elevated pressure and temperature Tsotsis, Thomas K.; Keller, Scott; Lee, Kyejune Composites Science and Technology, Vol. 61, Issue 1 https://doi.org/10.1016/S0266-3538(00)00196-2	journal	January 2001
Time development of diffusion-limited oxidation profiles in a radiation environment Wise, Jonathan; Gillen, Kenneth T.; Clough, Roger L. Radiation Physics and Chemistry, Vol. 49, Issue 5 https://doi.org/10.1016/S0969-806X(96)00185-5	journal	May 1997
Analysis of dual-mode model parameters for gas sorption in glassy polymers Kanehashi, Shinji; Nagai, Kazukiyo Journal of Membrane Science, Vol. 253, Issue 1-2 https://doi.org/10.1016/j.memsci.2005.01.003	journal	May 2005
Effect of oxygen pressure on the oxidation kinetics of unstabilised polypropylene Richaud, E.; Farcas, F.; Bartoloméo, P. Polymer Degradation and Stability, Vol. 91, Issue 2 https://doi.org/10.1016/j.polymdegradstab.2005.04.043	journal	February 2006
Accelerated aging and lifetime prediction: Review of non-Arrhenius behaviour due to two competing processes Celina, M.; Gillen, K. T.; Assink, R. A. Polymer Degradation and Stability, Vol. 90, Issue 3 https://doi.org/10.1016/j.polymdegradstab.2005.05.004	journal	December 2005
Review of polymer oxidation and its relationship with materials performance and lifetime prediction Celina, Mathew C. Polymer Degradation and Stability, Vol. 98, Issue 12 https://doi.org/10.1016/j.polymdegradstab.2013.06.024	journal	December 2013
Is carbonyl index a quantitative probe to monitor polypropylene photodegradation? Rouillon, C.; Bussiere, P. -O.; Desnoux, E. Polymer Degradation and Stability, Vol. 128 https://doi.org/10.1016/j.polymdegradstab.2015.12.011	journal	June 2016
Predictive ageing of elastomers: Oxidation driven modulus changes for polychloroprene Le Gac, Pierre Yves; Celina, Mathew; Roux, Gérard Polymer Degradation and Stability, Vol. 130 https://doi.org/10.1016/j.polymdegradstab.2016.06.014	journal	August 2016
Overview of DLO modeling and approaches to predict heterogeneous oxidative polymer degradation Quintana, Adam; Celina, Mathew C. Polymer Degradation and Stability, Vol. 149 https://doi.org/10.1016/j.polymdegradstab.2017.11.014	journal	March 2018
Multi-scale and multi-technical analysis of the thermal degradation of poly(ether imide) Courvoisier, Emilie; Bicaba, Yoann; Colin, Xavier Polymer Degradation and Stability, Vol. 147 https://doi.org/10.1016/j.polymdegradstab.2017.12.002	journal	January 2018
Multi-scale and multi-technique analysis of the thermal degradation of poly(ether ether ketone) Courvoisier, Emilie; Bicaba, Yoann; Colin, Xavier Polymer Degradation and Stability, Vol. 151 https://doi.org/10.1016/j.polymdegradstab.2018.03.001	journal	May 2018
Overview of accelerated aging and polymer degradation kinetics for combined radiation-thermal environments Celina, Mathew; Linde, Erik; Brunson, Douglas Polymer Degradation and Stability, Vol. 166 https://doi.org/10.1016/j.polymdegradstab.2019.06.007	journal	August 2019
Effect of UV-aging on the mechanical and fracture behavior of low density polyethylene Rodriguez, A. K.; Mansoor, B.; Ayoub, G. Polymer Degradation and Stability, Vol. 180 https://doi.org/10.1016/j.polymdegradstab.2020.109185	journal	October 2020
A new analytical model for predicting the thermal oxidation kinetics of composite organic m atrices. Application to diamine cross-linked epoxy Colin, Xavier; Essatbi, Fatima; Delozanne, Justine Polymer Degradation and Stability, Vol. 186 https://doi.org/10.1016/j.polymdegradstab.2021.109513	journal	April 2021
Carbonyl Identification and Quantification Uncertainties for Oxidative Polymer Degradation Celina, Mathew C.; Linde, Erik; Martinez, Estevan Polymer Degradation and Stability, Vol. 188 https://doi.org/10.1016/j.polymdegradstab.2021.109550	journal	June 2021
Time- and Feedback-Dependent DLO Phenomena in Oxidative Polymer Aging Linde, Erik; Nilsson, Fritjof; Barrett, Matija Polymer Degradation and Stability, Vol. 189 https://doi.org/10.1016/j.polymdegradstab.2021.109598	journal	July 2021
Use of a respirometer to measure oxidation rates of polymeric materials at ambient temperatures Assink, Roger A.; Celina, Mathew; Skutnik, Julie M. Polymer, Vol. 46, Issue 25 https://doi.org/10.1016/j.polymer.2005.09.069	journal	November 2005
A perspective on the inherent oxidation sensitivity of epoxy materials Celina, Mathew C.; Dayile, Angela R.; Quintana, Adam Polymer, Vol. 54, Issue 13 https://doi.org/10.1016/j.polymer.2013.04.042	journal	June 2013
Oxygen diffusivity and permeation through polymers at elevated temperature Celina, Mathew C.; Quintana, Adam Polymer, Vol. 150 https://doi.org/10.1016/j.polymer.2018.06.047	journal	August 2018
Dielectric spectroscopy as a condition monitoring technique for cable insulation based on crosslinked polyethylene Linde, E.; Verardi, L.; Fabiani, D. Polymer Testing, Vol. 44 https://doi.org/10.1016/j.polymertesting.2015.04.004	journal	July 2015
Origin of epoxies embrittlement during oxidative ageing Ernault, Esteve; Richaud, Emmanuel; Fayolle, Bruno Polymer Testing, Vol. 63 https://doi.org/10.1016/j.polymertesting.2017.09.004	journal	October 2017
Multi scale aging assessment of low-voltage cables subjected to radio-chemical aging: Towards an electrical diagnostic technique Suraci, Simone Vincenzo; Fabiani, Davide; Roland, Sébastien Polymer Testing, Vol. 103 https://doi.org/10.1016/j.polymertesting.2021.107352	journal	November 2021
The Oxidation of Unsaturated Compounds. VI. The Effect of Oxygen Pressure on the Oxidation of α-Methylstyrene^1,* Mayo, Frank R.; Miller, A. A. Journal of the American Chemical Society, Vol. 80, Issue 10 https://doi.org/10.1021/ja01543a031	journal	May 1958
Inhibition of Polyglycol Autoxidation. Lloyd, W. G. Journal of Chemical & Engineering Data, Vol. 6, Issue 4 https://doi.org/10.1021/je60011a019	journal	October 1961
Activation Barriers for Oxygen Diffusion in Polystyrene and Polycarbonate Glasses: Effects of Low Molecular Weight Additives Gao, Yuanping; Baca, Arthur M.; Wang, Bojie Macromolecules, Vol. 27, Issue 24 https://doi.org/10.1021/ma00102a006	journal	November 1994
Oxygen Permeability Measurements on Elastomers at Temperatures up to 225 °C Celina, M.; Gillen, K. T. Macromolecules, Vol. 38, Issue 7 https://doi.org/10.1021/ma0487913	journal	April 2005
Olefin oxidation Bateman, L. Quarterly Reviews, Chemical Society, Vol. 8, Issue 2 https://doi.org/10.1039/qr9540800147	journal	January 1954
Kinetic studies in the chemistry of rubber and related materials. II. The kinetics of oxidation of unconjugated olefins Bolland, J. L.; Gee, Geoffrey Transactions of the Faraday Society, Vol. 42 https://doi.org/10.1039/tf9464200236	journal	January 1946
Nuclear power plant cable materials : Celina, Mathias; Gillen, Kenneth; Lindgren, Eric https://doi.org/10.2172/1096518	report	May 2013
Transport Properdines of Gases in Polymers: Bibliographic Review Klopffer, M. H.; Flaconneche, B. Oil & Gas Science and Technology, Vol. 56, Issue 3 https://doi.org/10.2516/ogst:2001021	journal	May 2001
New Advances in the Kinetic Modeling of Thermal Oxidation of Epoxy-Diamine Networks Colin, Xavier; Delozanne, Justine; Moreau, Gurvan Frontiers in Materials, Vol. 8 https://doi.org/10.3389/fmats.2021.720455	journal	August 2021
Methods for Predicting More Confident Lifetimes of Seals in Air Environments Gillen, Kenneth T.; Celina, Mathias; Keenan, Michael R. Rubber Chemistry and Technology, Vol. 73, Issue 2 https://doi.org/10.5254/1.3547590	journal	May 2000
Thermal Degradation Studies of a Polyurethane Propellant Binder Celina, M.; Graham, A. C.; Gillen, K. T. Rubber Chemistry and Technology, Vol. 73, Issue 4 https://doi.org/10.5254/1.3547613	journal	September 2000
A Theoretical Model for the Diffusion-Limited Thermal Oxidation of Elastomers at Medium Temperatures Rincon-Rubio, L. M.; Colin, X.; Audouin, L. Rubber Chemistry and Technology, Vol. 76, Issue 2 https://doi.org/10.5254/1.3547754	journal	May 2003

Similar Records

Thermoset Blends of an Epoxy Resin and Polydicyclopentadiene

Journal Article · Tue Nov 29 23:00:00 EST 2016 · Macromolecules · OSTI ID:1337189

Coal tar autoxidation: kinetic studies by viscometric and refractometric methods

Conference · Wed Dec 31 23:00:00 EST 1975 · Am. Chem. Soc., Div. Fuel Chem., Prepr.; (United States) · OSTI ID:7348544

Morphology development of rubber-modified epoxy thermosets

Conference · Mon Dec 30 23:00:00 EST 1996 · OSTI ID:441492

Related Subjects

36 MATERIALS SCIENCE
Accelerated aging
DLO
Epoxy oxidation
O2 partial pressure
Rate behavior

Accelerated oxidation of epoxy thermosets with increased O2 pressure

Citation Formats

References (59)

Similar Records

Related Subjects

Accelerated oxidation of epoxy thermosets with increased O₂ pressure