Subdiffusive High-Pressure Hydrogen Gas Dynamics in Elastomers

Brownell, Matthew; Frischknecht, Amalie L.; Wilson, Mark A.

doi:10.1021/acs.macromol.2c00204

Title: Subdiffusive High-Pressure Hydrogen Gas Dynamics in Elastomers

Journal Article · Tue May 10 00:00:00 EDT 2022 · Macromolecules

DOI:https://doi.org/10.1021/acs.macromol.2c00204· OSTI ID:1877123

Brownell, Matthew ^[1];

^[1];

^[1]

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

We report elastomeric rubber materials serve a vital role as sealing materials in the hydrogen storage and transport infrastructure. With applications including O-rings and hose liners, these components are exposed to pressurized hydrogen at a range of temperatures, cycling rates, and pressure extremes. High-pressure exposure and subsequent rapid decompression often lead to cavitation and stress-induced damage of the elastomer due to localization of the hydrogen gas. Here, we use all-atom classical molecular dynamics simulations to assess the impact of compositional variations on gas diffusion within the commonly used elastomer ethylene–propylene–diene monomer (EPDM). With the aim to build a predictive understanding of precursors to cavitation and to motivate material formulations that are less sensitive to hydrogen-induced failure, we perform systematic simulations of gas dynamics in EPDM as a function of temperature, gas concentration, and cross-link density. Our simulations reveal anomalous, subdiffusive hydrogen motion at pressure and intermediate times. We identify two groups of gas with different mobilities: one group exhibiting high mobility and one group exhibiting low mobility due to their motion being impeded by the polymer. With decreasing temperatures, the low-mobility group shows increased gas localization, the necessary precursor for cavitation damage in these materials. At lower temperatures, increasing cross-link density led to greater hydrogen gas mobility and a lower fraction of caged hydrogen, indicating that increasing cross-link density may reduce precursors to cavitation. Finally, we use a two-state kinetic model to determine the energetics associated with transitions between these two mobility states.

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

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

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

OSTI ID:: 1877123

Report Number(s):: SAND2022-8320J; 707446

Journal Information:: Macromolecules, Vol. 55, Issue 10; ISSN 0024-9297

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (58)

Non-Gaussian nature of glassy dynamics by cage to cage motion Vorselaars, Bart; Lyulin, Alexey V.; Karatasos, K. Physical Review E, Vol. 75, Issue 1 https://doi.org/10.1103/PhysRevE.75.011504	journal	January 2007
The finite difference thermodynamic integration, tested on calculating the hydration free energy difference between acetone and dimethylamine in water Mezei, M. The Journal of Chemical Physics, Vol. 86, Issue 12 https://doi.org/10.1063/1.452357	journal	June 1987
Predictive calculation of hydrogen and helium solubility in glassy and rubbery polymers Galizia, Michele; Smith, Zachary P.; Sarti, Giulio C. Journal of Membrane Science, Vol. 475 https://doi.org/10.1016/j.memsci.2014.10.009	journal	February 2015
Hydrogen from solar energy, a clean energy carrier from a sustainable source of energy Hosseini, Seyed Ehsan; Wahid, Mazlan Abdul International Journal of Energy Research, Vol. 44, Issue 6 https://doi.org/10.1002/er.4930	journal	May 2020
Temperature-Dependent Elasticity of a Semicrystalline Interphase Composed of Freely Rotating Chains in 't Veld, Pieter J.; Rutledge, Gregory C. Macromolecules, Vol. 36, Issue 19 https://doi.org/10.1021/ma0346658	journal	September 2003
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
Non-dimensional assessments to estimate decompression failure in polymers for hydrogen systems Melnichuk, Maximiliano; Thiébaud, Frédéric; Perreux, Dominique International Journal of Hydrogen Energy, Vol. 45, Issue 11 https://doi.org/10.1016/j.ijhydene.2019.12.107	journal	February 2020
Numerical integration of the cartesian equations of motion of a system with constraints: molecular dynamics of n-alkanes Ryckaert, Jean-Paul; Ciccotti, Giovanni; Berendsen, Herman J. C. Journal of Computational Physics, Vol. 23, Issue 3 https://doi.org/10.1016/0021-9991(77)90098-5	journal	March 1977
Hybrid fuel cell system degradation modeling methods: A comprehensive review Vichard, L.; Steiner, N. Yousfi; Zerhouni, N. Journal of Power Sources, Vol. 506 https://doi.org/10.1016/j.jpowsour.2021.230071	journal	September 2021
A Review on Applicability, Limitations, and Improvements of Polymeric Materials in High-Pressure Hydrogen Gas Atmospheres Balasooriya, Winoj; Clute, Clara; Schrittesser, Bernd Polymer Reviews, Vol. 62, Issue 1 https://doi.org/10.1080/15583724.2021.1897997	journal	March 2021
Super Gas Barrier of All-Polymer Multilayer Thin Films Yang, You-Hao; Haile, Merid; Park, Yong Tae Macromolecules, Vol. 44, Issue 6 https://doi.org/10.1021/ma1026127	journal	March 2011
Reinforcement of elastomers Heinrich, Gert; Klüppel, Manfred; Vilgis, Thomas A. Current Opinion in Solid State and Materials Science, Vol. 6, Issue 3 https://doi.org/10.1016/S1359-0286(02)00030-X	journal	June 2002
Fast Parallel Algorithms for Short-Range Molecular Dynamics Plimpton, Steve Journal of Computational Physics, Vol. 117, Issue 1 https://doi.org/10.1006/jcph.1995.1039	journal	March 1995
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
Transport dynamics of complex fluids Song, Sanggeun; Park, Seong Jun; Kim, Minjung Proceedings of the National Academy of Sciences, Vol. 116, Issue 26 https://doi.org/10.1073/pnas.1900239116	journal	June 2019
Evaluation on High-Pressure Hydrogen Decompression Failure of Rubber O-ring Using Design of Experiments Koga, Atsushi; Uchida, Kenichi; Yamabe, Junichiro International Journal of Automotive Engineering, Vol. 2, Issue 4 https://doi.org/10.20485/jsaeijae.2.4_123	journal	January 2011
Coarse-Grained Molecular Simulation of Penetrant Diffusion in a Glassy Polymer Using Reverse and Kinetic Monte Carlo Greenfield, Michael L.; Theodorou, Doros N. Macromolecules, Vol. 34, Issue 24 https://doi.org/10.1021/ma002157h	journal	October 2001
Reinforcement of EPDM rubber with in situ generated silica particles in the presence of a coupling agent via a sol–gel route Mokhothu, T. H.; Luyt, A. S.; Messori, M. Polymer Testing, Vol. 33 https://doi.org/10.1016/j.polymertesting.2013.11.009	journal	February 2014
Anomalous yet Brownian Wang, B.; Anthony, S. M.; Bae, S. C. Proceedings of the National Academy of Sciences, Vol. 106, Issue 36 https://doi.org/10.1073/pnas.0903554106	journal	July 2009
Fickian yet non-Gaussian diffusion in two-dimensional Yukawa liquids Ghannad, Zahra Physical Review E, Vol. 100, Issue 3 https://doi.org/10.1103/PhysRevE.100.033211	journal	September 2019
Nanoparticle Mobility within Permanently Cross-Linked Polymer Networks Chen, Yulong; Ma, Rui; Qian, Xin Macromolecules, Vol. 53, Issue 11 https://doi.org/10.1021/acs.macromol.0c00334	journal	May 2020
Development of high pressure gaseous hydrogen storage technologies Zheng, Jinyang; Liu, Xianxin; Xu, Ping International Journal of Hydrogen Energy, Vol. 37, Issue 1 https://doi.org/10.1016/j.ijhydene.2011.02.125	journal	January 2012
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
On key parameters influencing cavitation damage upon fast decompression in a hydrogen saturated elastomer Jaravel, Julien; Castagnet, Sylvie; Grandidier, Jean-Claude Polymer Testing, Vol. 30, Issue 8 https://doi.org/10.1016/j.polymertesting.2011.08.003	journal	December 2011
Computer Simulation of Liquids. Scott, R.; Allen, M. P.; Tildesley, D. J. Mathematics of Computation, Vol. 57, Issue 195 https://doi.org/10.2307/2938686	journal	July 1991
The glass transition temperature of PMMA: A molecular dynamics study and comparison of various determination methods Mohammadi, Maryam; fazli, Hossein; karevan, Mehdi European Polymer Journal, Vol. 91 https://doi.org/10.1016/j.eurpolymj.2017.03.056	journal	June 2017
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
COMPASS: An ab Initio Force-Field Optimized for Condensed-Phase ApplicationsOverview with Details on Alkane and Benzene Compounds Sun, H. The Journal of Physical Chemistry B, Vol. 102, Issue 38 https://doi.org/10.1021/jp980939v	journal	September 1998
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
Brownian yet Non-Gaussian Diffusion: From Superstatistics to Subordination of Diffusing Diffusivities Chechkin, Aleksei V.; Seno, Flavio; Metzler, Ralf Physical Review X, Vol. 7, Issue 2 https://doi.org/10.1103/PhysRevX.7.021002	journal	April 2017
Molecular simulations of gas transport in hydrogenated nitrile butadiene rubber and ethylene–propylene–diene rubber Tan, JingHua; Chen, Chenliang; Liu, Yiwu RSC Advances, Vol. 10, Issue 21 https://doi.org/10.1039/D0RA00192A	journal	January 2020
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 Storage for Mobility: A Review Rivard, Etienne; Trudeau, Michel; Zaghib, Karim Materials, Vol. 12, Issue 12 https://doi.org/10.3390/ma12121973	journal	June 2019
Development and Testing of the OPLS All-Atom Force Field on Conformational Energetics and Properties of Organic Liquids Jorgensen, William L.; Maxwell, David S.; Tirado-Rives, Julian Journal of the American Chemical Society, Vol. 118, Issue 45 https://doi.org/10.1021/ja9621760	journal	January 1996
Influence of Polymer Motion, Topology and Simulation Size on Penetrant Diffusion in Amorphous, Glassy Polymers: Diffusion of Helium in Polypropylene Boshoff, Jan H. D.; Lobo, Raul F.; Wagner, Norman J. Macromolecules, Vol. 34, Issue 17 https://doi.org/10.1021/ma010255c	journal	July 2001
Influence of ethylene–propylene ratio on the thermal degradation behaviour of EPDM elastomers Gamlin, Clint; Dutta, Naba; Roy-Choudhury, Namita Thermochimica Acta, Vol. 367-368 https://doi.org/10.1016/S0040-6031(00)00668-7	journal	March 2001
Gas transport in ethylene–propylene–diene (EPDM) elastomer: Molecular simulation and experimental study Rutherford, S. W.; Limmer, D. T.; Smith, M. G. Polymer, Vol. 48, Issue 22 https://doi.org/10.1016/j.polymer.2007.07.020	journal	October 2007
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
Determination of key parameters responsible for polymeric liner collapse in hyperbaric type IV hydrogen storage vessels Pepin, Julie; Lainé, Eric; Grandidier, Jean-Claude International Journal of Hydrogen Energy, Vol. 43, Issue 33 https://doi.org/10.1016/j.ijhydene.2018.06.177	journal	August 2018
“Explosive Decompression Failure” of Rubbers: A Review of the Origins of Pneumatic Stress Induced Rupture in Elastomers Briscoe, B. J.; Savvas, T.; Kelly, C. T. Rubber Chemistry and Technology, Vol. 67, Issue 3 https://doi.org/10.5254/1.3538683	journal	July 1994
Influence of Structure of Elastomers on Their Permeability to Gases Van Amerongen, G. J. Rubber Chemistry and Technology, Vol. 24, Issue 1 https://doi.org/10.5254/1.3543028	journal	March 1951
Computational evidence for anomalous diffusion of small molecules in amorphous polymers Müller-Plathe, Florian; Rogers, Stephen C.; van Gunsteren, Wilfred F. Chemical Physics Letters, Vol. 199, Issue 3-4 https://doi.org/10.1016/0009-2614(92)80112-O	journal	November 1992
The Permeability of Different Rubbers to Gases and Its Relation to Diffusivity and Solubility Van Amerongen, G. J. Journal of Applied Physics, Vol. 17, Issue 11 https://doi.org/10.1063/1.1707667	journal	November 1946
Predicting the glass transition temperature as function of crosslink density and polymer interactions in rubber compounds D’Escamard, Gabriella; De Rosa, Claudio; Auriemma, Finizia VIII INTERNATIONAL CONFERENCE ON “TIMES OF POLYMERS AND COMPOSITES”: From Aerospace to Nanotechnology, AIP Conference Proceedings https://doi.org/10.1063/1.4949751	conference	January 2016
An in situ tribometer for measuring friction and wear of polymers in a high pressure hydrogen environment Duranty, Edward R.; Roosendaal, Timothy J.; Pitman, Stan G. Review of Scientific Instruments, Vol. 88, Issue 9 https://doi.org/10.1063/1.5001836	journal	September 2017
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
Thermo-oxidative degradation of a carbon black compounded EPDM rubber hose Kwak, S. B.; Choi, N. S. International Journal of Automotive Technology, Vol. 12, Issue 3 https://doi.org/10.1007/s12239-011-0047-3	journal	May 2011
Permeation of polymers — a computational approach Müller-Plathe, Florian Acta Polymerica, Vol. 45, Issue 4, p. 259-293 https://doi.org/10.1002/actp.1994.010450401	journal	July 1994
Molecular dynamics simulations of diffusion of small molecules in polymers: Effect of chain length Takeuchi, Hisao The Journal of Chemical Physics, Vol. 93, Issue 6 https://doi.org/10.1063/1.458689	journal	September 1990
21st Century’s energy: Hydrogen energy system Veziroğlu, T. Nejat; Şahi˙n, Sümer Energy Conversion and Management, Vol. 49, Issue 7, p. 1820-1831 https://doi.org/10.1016/j.enconman.2007.08.015	journal	July 2008
LAMMPS - a flexible simulation tool for particle-based materials modeling at the atomic, meso, and continuum scales Thompson, Aidan P.; Aktulga, H. Metin; Berger, Richard Computer Physics Communications, Vol. 271 https://doi.org/10.1016/j.cpc.2021.108171	journal	February 2022
Transport of probe particles in a polymer network: effects of probe size, network rigidity and probe–polymer interaction Kumar, Praveen; Theeyancheri, Ligesh; Chaki, Subhasish Soft Matter, Vol. 15, Issue 44 https://doi.org/10.1039/C9SM01822K	journal	January 2019
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
Correlations in Space and Time and Born Approximation Scattering in Systems of Interacting Particles Van Hove, Léon Physical Review, Vol. 95, Issue 1 https://doi.org/10.1103/PhysRev.95.249	journal	July 1954
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 Network Structure on Glass Transition Temperature of Elastomers Bandzierz, Katarzyna; Reuvekamp, Louis; Dryzek, Jerzy Materials, Vol. 9, Issue 7 https://doi.org/10.3390/ma9070607	journal	July 2016
Hydrogen damage of steels: A case study and hydrogen embrittlement model Djukic, M. B.; Sijacki Zeravcic, V.; Bakic, G. M. Engineering Failure Analysis, Vol. 58 https://doi.org/10.1016/j.engfailanal.2015.05.017	journal	December 2015
Hydrogen embrittlement of metals Louthan, M. R.; Caskey, G. R.; Donovan, J. A. Materials Science and Engineering, Vol. 10 https://doi.org/10.1016/0025-5416(72)90109-7	journal	January 1972

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