Multi-scale imaging of high-pressure hydrogen induced damage in EPDM rubber using X-ray microcomputed tomography, helium-ion microscopy and transmission electron microscopy

Kuang, Wenbin; Arey, Bruce W.; Dohnalkova, Alice C.; Kovarik, Libor; Mills, Bernice; Menon, Nalini C.; Seffens, Robert J.; Simmons, Kevin L.

doi:10.1016/j.ijhydene.2022.12.004

Multi-scale imaging of high-pressure hydrogen induced damage in EPDM rubber using X-ray microcomputed tomography, helium-ion microscopy and transmission electron microscopy

Journal Article · Sat Dec 17 00:00:00 EST 2022 · International Journal of Hydrogen Energy

DOI:https://doi.org/10.1016/j.ijhydene.2022.12.004· OSTI ID:1962331

Kuang, Wenbin ^[1]; Arey, Bruce W. ^[1]; Dohnalkova, Alice C. ^[1]; Kovarik, Libor ^[1]; Mills, Bernice ^[2]; Menon, Nalini C. ^[2]; Seffens, Robert J. ^[1]; Simmons, Kevin L. ^[1]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sandia National Lab. (SNL-CA), Livermore, CA (United States)

Ethylene propylene diene (EPDM) rubber has gained increasing interest for use in hydrogen infrastructure due to its excellent sealing performance and low temperature properties. However, severe structural damage has been observed in EPDM O-rings after exposure to high-pressure hydrogen. The origination and propagation mechanisms of this damage are poorly understood. Here, to address this knowledge gap, multi-scale imaging leveraging X-ray micro-computed tomography (micro-CT), helium ion microscopy (HeIM), and transmission electron microscopy (TEM) were used in this work to study a series of sulfur-cured ethylene propylene diene (EPDM) rubber materials with varying additives that were exposed to different hydrogen environments. Micro-CT captured the substantial structural damage due to hydrogen exposure; it revealed an association between zinc oxide (ZnO) particles and damage initiation. Further studies by TEM and scanning TEM with energy dispersive X-ray spectroscopy (EDS) were focused on these particles at the micro-to nano-scale range. TEM indicated that hydrogen causes void formation at the interface between ZnO and the rubber matrix. HeIM enabled imaging of surface morphology of the material at high resolution pre- and post-hydrogen exposure while providing information on chemical composition and that cannot be captured by either micro-CT or TEM.

View Accepted Manuscript (DOE)

Research Organization:: Environmental Molecular Sciences Laboratory (EMSL), Richland, WA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Sandia National Laboratories (SNL-CA), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Hydrogen Fuel Cell Technologies Office (HFTO); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830; NA0003525

OSTI ID:: 1962331

Report Number(s):: PNNL-SA-177303

Journal Information:: International Journal of Hydrogen Energy, Journal Name: International Journal of Hydrogen Energy Journal Issue: 23 Vol. 48; ISSN 0360-3199

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (48)

Recent Advances in the Study of Structural Materials Compatibility with Hydrogen Dadfarnia, M.; Novak, P.; Ahn, D. C. Advanced Materials, Vol. 22, Issue 10 https://doi.org/10.1002/adma.200904354	journal	March 2010
Visualization of surface and subsurface morphology: The effect of processing on a rubber-modified thermoplastic Edwards, S. A.; Roy Choudhury, N.; Provatas, M. Journal of Applied Polymer Science, Vol. 87, Issue 5 https://doi.org/10.1002/app.11443	journal	December 2002
The determination of zinc oxide in rubber vulcanizates by x-ray diffraction Laning, Stephen H.; Wagner, Melvin P.; Sellers, John W. Journal of Applied Polymer Science, Vol. 2, Issue 5 https://doi.org/10.1002/app.1959.070020517	journal	September 1959
Influence of zinc oxide during different stages of sulfur vulcanization. Elucidated by model compound studies Heideman, G.; Datta, R. N.; Noordermeer, J. W. M. Journal of Applied Polymer Science, Vol. 95, Issue 6 https://doi.org/10.1002/app.21364	journal	January 2005
Application of nano-zinc oxide master batch in polybutadiene styrene rubber system Jincheng, Wang; Yuehui, Chen Journal of Applied Polymer Science, Vol. 101, Issue 2 https://doi.org/10.1002/app.23983	journal	January 2006
Effect of zinc oxide nanoparticles as cure activator on the properties of natural rubber and nitrile rubber Sahoo, Suchismita; Maiti, Madhuchhanda; Ganguly, Anirban Journal of Applied Polymer Science, Vol. 105, Issue 4 https://doi.org/10.1002/app.26296	journal	January 2007
Influence of carbon black on decompression failure and hydrogen permeation properties of filled ethylene-propylene-diene-methylene rubbers exposed to high-pressure hydrogen gas Yamabe, Junichiro; Nishimura, Shin Journal of Applied Polymer Science, Vol. 122, Issue 5 https://doi.org/10.1002/app.34344	journal	July 2011
Multi‐Scale Imaging of Polymer Electrolyte Fuel Cells using X‐ray Micro‐ and Nano‐Computed Tomography, Transmission Electron Microscopy and Helium‐Ion Microscopy Meyer, Q.; Hack, J.; Mansor, N. Fuel Cells, Vol. 19, Issue 1 https://doi.org/10.1002/fuce.201800047	journal	January 2019
Nanoscale fracture analysis by atomic force microscopy of EPDM rubber due to high-pressure hydrogen decompression Yamabe, Junichiro; Nishimura, Shin Journal of Materials Science, Vol. 46, Issue 7 https://doi.org/10.1007/s10853-010-5073-4	journal	November 2010
Detection of hydrogen dissolved in acrylonitrile butadiene rubber by 1H nuclear magnetic resonance Nishimura, Shin; Fujiwara, Hirotada Chemical Physics Letters, Vol. 522 https://doi.org/10.1016/j.cplett.2011.11.080	journal	January 2012
Failure behavior of rubber O-ring under cyclic exposure to high-pressure hydrogen gas Yamabe, Junichiro; koga, Atsushi; Nishimura, Shin Engineering Failure Analysis, Vol. 35 https://doi.org/10.1016/j.engfailanal.2013.01.034	journal	December 2013
Influence of fillers on hydrogen penetration properties and blister fracture of rubber composites for O-ring exposed to high-pressure hydrogen gas Yamabe, Junichiro; Nishimura, Shin International Journal of Hydrogen Energy, Vol. 34, Issue 4 https://doi.org/10.1016/j.ijhydene.2008.11.105	journal	February 2009
Evaluation of the change in chemical structure of acrylonitrile butadiene rubber after high-pressure hydrogen exposure Fujiwara, Hirotada; Yamabe, Junichiro; Nishimura, Shin International Journal of Hydrogen Energy, Vol. 37, Issue 10 https://doi.org/10.1016/j.ijhydene.2012.02.084	journal	May 2012
Perspective on hydrogen energy carrier and its automotive applications Cipriani, Giovanni; Di Dio, Vincenzo; Genduso, Fabio International Journal of Hydrogen Energy, Vol. 39, Issue 16 https://doi.org/10.1016/j.ijhydene.2014.03.174	journal	May 2014
Development of methods for evaluating hydrogen compatibility and suitability San Marchi, Chris; Somerday, Brian P.; Nibur, Kevin A. International Journal of Hydrogen Energy, Vol. 39, Issue 35 https://doi.org/10.1016/j.ijhydene.2014.03.234	journal	December 2014
Inhomogeneity in acrylonitrile butadiene rubber during hydrogen elimination investigated by small-angle X-ray scattering Ohyama, Keiko; Fujiwara, Hirotada; Nishimura, Shin International Journal of Hydrogen Energy, Vol. 43, Issue 2 https://doi.org/10.1016/j.ijhydene.2017.10.162	journal	January 2018
Hydrogen energy, economy and storage: Review and recommendation Abe, J. O.; Popoola, A. P. I.; Ajenifuja, E. International Journal of Hydrogen Energy, Vol. 44, Issue 29 https://doi.org/10.1016/j.ijhydene.2019.04.068	journal	June 2019
A review on effect of hydrogen on rubber seals used in the high-pressure hydrogen infrastructure Zheng, Yiran; Tan, Yue; Zhou, Chilou International Journal of Hydrogen Energy, Vol. 45, Issue 43 https://doi.org/10.1016/j.ijhydene.2020.06.069	journal	September 2020
H-Mat hydrogen compatibility of polymers and elastomers Simmons, K. L.; Kuang, W.; Burton, S. D. International Journal of Hydrogen Energy, Vol. 46, Issue 23 https://doi.org/10.1016/j.ijhydene.2020.06.218	journal	March 2021
Damage evolution in polymer due to exposure to high-pressure hydrogen gas Kulkarni, Shank S.; Choi, Kyoo Sil; Kuang, Wenbin International Journal of Hydrogen Energy, Vol. 46, Issue 36 https://doi.org/10.1016/j.ijhydene.2021.03.035	journal	May 2021
Effects of fillers on the hydrogen uptake and volume expansion of acrylonitrile butadiene rubber composites exposed to high pressure hydrogen: -Property of polymeric materials for high pressure hydrogen devices (3)- Fujiwara, Hirotada; Ono, Hiroaki; Nishimura, Shin International Journal of Hydrogen Energy, Vol. 47, Issue 7 https://doi.org/10.1016/j.ijhydene.2021.11.061	journal	January 2022
High-pressure hydrogen decompression in sulfur crosslinked elastomers Wilson, Mark A.; Frischknecht, Amalie L. International Journal of Hydrogen Energy, Vol. 47, Issue 33 https://doi.org/10.1016/j.ijhydene.2022.03.015	journal	April 2022
Effect of zinc oxide type on ageing properties of Styrene Butadiene Rubber compounds Vatansever, Nurhan; Polat, Şeyda Materials & Design, Vol. 31, Issue 3 https://doi.org/10.1016/j.matdes.2009.09.015	journal	March 2010
Investigation of cure behaviour and tensile properties of NR/SBR composite filled with carbon black and silica Seshaiah, Nagam; Santhosh Kumar, Narava; Khadar Hussain Afrid, Mahamad Materials Today: Proceedings, Vol. 59 https://doi.org/10.1016/j.matpr.2021.11.352	journal	January 2022
Reinforcement of natural rubber with silica/carbon black hybrid filler Rattanasom, N.; Saowapark, T.; Deeprasertkul, C. Polymer Testing, Vol. 26, Issue 3 https://doi.org/10.1016/j.polymertesting.2006.12.003	journal	May 2007
Application of acoustic emission method to detection of internal fracture of sealing rubber material by high-pressure hydrogen decompression Yamabe, Junichiro; Matsumoto, Takashi; Nishimura, Shin Polymer Testing, Vol. 30, Issue 1 https://doi.org/10.1016/j.polymertesting.2010.11.002	journal	February 2011
In-situ X-ray computed tomography of decompression failure in a rubber exposed to high-pressure gas Castagnet, Sylvie; Mellier, David; Nait-Ali, Azdine Polymer Testing, Vol. 70 https://doi.org/10.1016/j.polymertesting.2018.07.017	journal	September 2018
Rapid Gas Decompression Performance of elastomers – A study of influencing testing parameters Schrittesser, B.; Pinter, G.; Schwarz, Th. Procedia Structural Integrity, Vol. 2 https://doi.org/10.1016/j.prostr.2016.06.220	journal	January 2016
On hydrogen and hydrogen energy strategies Midilli, A.; Ay, M.; Dincer, I. Renewable and Sustainable Energy Reviews, Vol. 9, Issue 3 https://doi.org/10.1016/j.rser.2004.05.003	journal	June 2005
A review on the role, cost and value of hydrogen energy systems for deep decarbonisation Parra, David; Valverde, Luis; Pino, F. Javier Renewable and Sustainable Energy Reviews, Vol. 101 https://doi.org/10.1016/j.rser.2018.11.010	journal	March 2019
Wind energy and the hydrogen economy—review of the technology Sherif, S. A.; Barbir, F.; Veziroglu, T. N. Solar Energy, Vol. 78, Issue 5 https://doi.org/10.1016/j.solener.2005.01.002	journal	May 2005
Formation of an adsorption film of MoS2 nanoparticles and dioctyl sebacate on a steel surface for alleviating friction and wear Xu, Yong; Hu, Enzhu; Hu, Kunhong Tribology International, Vol. 92 https://doi.org/10.1016/j.triboint.2015.06.011	journal	December 2015
In situ friction and wear behavior of rubber materials incorporating various fillers and/or a plasticizer in high-pressure hydrogen Kuang, Wenbin; Bennett, Wendy D.; Roosendaal, Timothy J. Tribology International, Vol. 153 https://doi.org/10.1016/j.triboint.2020.106627	journal	January 2021
Microsized Pore Structure Determination in EPDM Rubbers Using High-Pressure ¹²⁹Xe NMR Techniques Han, Kee Sung; Burton, Sarah D.; Walter, Eric D. The Journal of Physical Chemistry B, Vol. 126, Issue 16 https://doi.org/10.1021/acs.jpcb.1c09189	journal	April 2022
Subdiffusive High-Pressure Hydrogen Gas Dynamics in Elastomers Brownell, Matthew; Frischknecht, Amalie L.; Wilson, Mark A. Macromolecules, Vol. 55, Issue 10 https://doi.org/10.1021/acs.macromol.2c00204	journal	May 2022
Evaluation of hydrogen dissolved in rubber materials under high-pressure exposure using nuclear magnetic resonance Fujiwara, Hirotada; Nishimura, Shin Polymer Journal, Vol. 44, Issue 8 https://doi.org/10.1038/pj.2012.111	journal	June 2012
Evaluating the effect of processing parameters on the replication quality in the micro compression molding of silicone rubber Maghsoudi, Khosrow; Vazirinasab, E.; Jafari, R. Materials and Manufacturing Processes, Vol. 35, Issue 14 https://doi.org/10.1080/10426914.2020.1779942	journal	June 2020
Effect of processing parameters on the vulcanisation of natural rubber using glutaraldehyde Kalkornsurapranee, Ekwipoo; Yung-Aoon, Wanida; Songtipya, Ladawan Plastics, Rubber and Composites, Vol. 46, Issue 6 https://doi.org/10.1080/14658011.2017.1323610	journal	May 2017
Development of material formula and structure property indicators for low cold-resistant characterization of Cables’ Material Sun, W.; Cai, Y. G.; Feng, Y. M. IOP Conference Series: Materials Science and Engineering, Vol. 292 https://doi.org/10.1088/1757-899X/292/1/012066	journal	January 2018
Influence of Carbon Black on Crack Damage of Sealing Rubber Material Exposed to High-Pressure Hydrogen Gas Yamabe, Junichiro; Nishimura, Shin TRANSACTIONS OF THE JAPAN SOCIETY OF MECHANICAL ENGINEERS Series A, Vol. 77, Issue 774 https://doi.org/10.1299/kikaia.77.323	journal	January 2011
Evaluating the effect of processing conditions and organoclay content on the properties of styrene-butadiene rubber/organoclay nanocomposites by response surface methodology Ghasemi, I.; Karrabi, M.; Mohammadi, M. Express Polymer Letters, Vol. 4, Issue 2 https://doi.org/10.3144/expresspolymlett.2010.11	journal	January 2010
Nature of Carbon Black Reinforcement of Rubber: Perspective on the Original Polymer Nanocomposite Robertson, Christopher G.; Hardman, Ned J. Polymers, Vol. 13, Issue 4 https://doi.org/10.3390/polym13040538	journal	February 2021
Filler Influence on H2 Permeation Properties in Sulfur-CrossLinked Ethylene Propylene Diene Monomer Polymers Blended with Different Concentrations of Carbon Black and Silica Fillers Jung, Jae Kap; Lee, Chang Hoon; Baek, Un Bong Polymers, Vol. 14, Issue 3 https://doi.org/10.3390/polym14030592	journal	February 2022
Effect of Functional Fillers on Tribological Characteristics of Acrylonitrile Butadiene Rubber after High-Pressure Hydrogen Exposures Choi, Byeong-Lyul; Jung, Jae; Baek, Un Polymers, Vol. 14, Issue 5 https://doi.org/10.3390/polym14050861	journal	February 2022
The Effects of Carbon Black-Vulcanization System Interactions on Natural Rubber Network Structures and Properties Pal, P. K.; Bhowmick, A. K.; De, S. K. Rubber Chemistry and Technology, Vol. 55, Issue 1 https://doi.org/10.5254/1.3535871	journal	March 1982
The Effect of Fillers on the Permeability of Rubber to Gases Van Amerongen, G. J. Rubber Chemistry and Technology, Vol. 28, Issue 3 https://doi.org/10.5254/1.3542844	journal	September 1955
Bonding of Rubber to Carbon Black by Sulfur Vulcanization Rivin, D.; Aron, J.; Medalia, A. I. Rubber Chemistry and Technology, Vol. 41, Issue 2 https://doi.org/10.5254/1.3547172	journal	May 1968
Influence of Filler Particle Size on Behaviour of EPDM Rubber for Fuel Cell Vehicle Application under High-Pressure Hydrogen Environment Kim, Keejung; Jeon, Hyeong-Ryeol; Kang, Young-Im Transctions of the Korean Hydrogen and New Energy Society, Vol. 31, Issue 5 https://doi.org/10.7316/KHNES.2020.31.5.453	journal	October 2020

Similar Records

Deuterium permeation through EPDM rubber compounds

Conference · Thu Dec 31 23:00:00 EST 1987 · OSTI ID:6669223

Response of ethylene propylene diene monomer rubber (EPDM) to simulant Hanford tank waste

Technical Report · Mon Jan 31 23:00:00 EST 2000 · OSTI ID:752052

Atomistic Materials Modeling of High-Pressure Hydrogen Interactions in Ethylene Propylene Diene Monomer (EPDM) Rubber

Technical Report · Tue Nov 01 00:00:00 EDT 2022 · OSTI ID:1898282

Related Subjects

08 HYDROGEN
helium ion microscopy
hydrogen degradation
micro-computed tomography
rubber
transmission electron microscopy

Multi-scale imaging of high-pressure hydrogen induced damage in EPDM rubber using X-ray microcomputed tomography, helium-ion microscopy and transmission electron microscopy

Citation Formats

References (48)

Similar Records

Related Subjects