Molecular Dynamics Simulation of Hygroscopic Aging Effects in Epoxy Polymer

Taufique, Mohammad F. N.; Losada, Martin; Hamel, Sebastien; Goldman, Nir; DiTucci, Matthew J.; Pagnotti, Loubna; Willis, Daniel; Torres, Matthew; Devanathan, Ram

doi:10.1007/s40192-023-00296-5

Title: Molecular Dynamics Simulation of Hygroscopic Aging Effects in Epoxy Polymer

Journal Article · 31 July 2023 · Integrating Materials and Manufacturing Innovation

DOI: https://doi.org/10.1007/s40192-023-00296-5 · OSTI ID:2045602

^[1]; Losada, Martin ^[2]; Hamel, Sebastien ^[3]; Goldman, Nir ^[3]; DiTucci, Matthew J. ^[2]; Pagnotti, Loubna ^[2]; Willis, Daniel ^[2]; Torres, Matthew ^[2];

^[1]

Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
PPG Coatings Innovation Center, Allison Park, PA (United States)
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

The automobile industry is incorporating more lightweight content in car designs to boost fuel-economy. New structural adhesives are needed to mitigate the corrosion and thermal expansion issues associated with joining dissimilar lightweight materials, but adhesive developers lack a fundamental understanding of the chemistry that occurs in the adhesive as the joint ages. In this study, we developed structural adhesive molecular models and applied classical molecular dynamics simulations and density functional theory calculations to gain molecular insights into the influence of water molecules on the properties of epoxy-based adhesives (DGEBA + Jeffamine (JD230)). The simulations were complemented by experimental synthesis and characterization. Our work underscores the impact of water molecules on the local structure of the epoxy network as well as resulting mechanical properties. Water molecules were mainly coordinated with hydroxyls, primary amines and secondary amines, but also weakly coordinated with ether linkages, which were found most probable to be labile. Simulated stress–strain data indicates that increasing the water content deteriorates the mechanical properties. The Young’s modulus decreased by ~ 30% when the water content increased to 3 wt%. We conclude, this integration of molecular-level chemical insights with mechanical property simulations of the hydrated epoxy system and experimental validation holds the promise to advance lightweight joint technologies.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC05-76RL01830; AC02-05CH11231; AC52-07NA27344

OSTI ID:: 2045602

Report Number(s):: PNNL-SA--161079; LLNL--JRNL-821077

Journal Information:: Integrating Materials and Manufacturing Innovation, Journal Name: Integrating Materials and Manufacturing Innovation Journal Issue: 3 Vol. 12; ISSN 2193-9764

Publisher:: SpringerCopyright Statement

Country of Publication:: United States

Language:: English

References (59)

Contributions of the nanovoid structure to the moisture absorption properties of epoxy resins Soles, Christopher L.; Chang, Fernando T.; Bolan, Brett A. Journal of Polymer Science Part B: Polymer Physics, Vol. 36, Issue 17 https://doi.org/10.1002/(SICI)1099-0488(199812)36:17<3035::AID-POLB4>3.0.CO;2-Y	journal	December 1998
The effect of the prepolymer composition of amino-hardened epoxy resins on the water sorption behavior and plasticization Carfagna, C.; Apicella, A.; Nicolais, L. Journal of Applied Polymer Science, Vol. 27, Issue 1 https://doi.org/10.1002/app.1982.070270112	journal	January 1982
PACKMOL: A package for building initial configurations for molecular dynamics simulations Martínez, L.; Andrade, R.; Birgin, E. G. Journal of Computational Chemistry, Vol. 30, Issue 13 https://doi.org/10.1002/jcc.21224	journal	October 2009
Application of molecular dynamics simulations in molecular property prediction II: Diffusion coefficient Wang, Junmei; Hou, Tingjun Journal of Computational Chemistry, Vol. 32, Issue 16 https://doi.org/10.1002/jcc.21939	journal	September 2011
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
The application of differential scanning calorimetry (DSC) to the study of epoxy resin curing reactions Barton, John M. Advances in Polymer Science https://doi.org/10.1007/3-540-15546-5_5	book	January 1985
Polymer Nanocomposites: Emerging Growth Driver for the Global Automotive Industry Patel, Vivek; Mahajan, Yashwant Handbook of Polymernanocomposites. Processing, Performance and Application https://doi.org/10.1007/978-3-642-38649-7_23	book	December 2013
Coatings and other applications of epoxy resins Chen, X. M.; Ellis, B. Chemistry and Technology of Epoxy Resins https://doi.org/10.1007/978-94-011-2932-9_9	book	January 1993
Thermodynamic and mechanical properties of amine-cured epoxy resins using group interaction modelling Foreman, Joel P.; Porter, David; Behzadi, Shabnam Journal of Materials Science, Vol. 41, Issue 20 https://doi.org/10.1007/s10853-006-0202-9	journal	August 2006
Molecular dynamics approach on the hygroelastic behavior of epoxy/graphene nanocomposites Kwon, Sunyong; Lee, Man Young; Yang, Seunghwa Journal of Mechanical Science and Technology, Vol. 33, Issue 2 https://doi.org/10.1007/s12206-019-0128-1	journal	February 2019
Research trends in polymer materials for use in lightweight vehicles Lyu, Min-Young; Choi, Tae Gyun International Journal of Precision Engineering and Manufacturing, Vol. 16, Issue 1 https://doi.org/10.1007/s12541-015-0029-x	journal	January 2015
The effect of stoichiometry and thermal history during cure on structure and properties of epoxy networks Meyer, Fred; Sanz, Genoveva; Eceiza, Arantxa Polymer, Vol. 36, Issue 7 https://doi.org/10.1016/0032-3861(95)95918-Q	journal	March 1995
The potential for composites in structural automotive applications Beardmore, P.; Johnson, C. F. Composites Science and Technology, Vol. 26, Issue 4 https://doi.org/10.1016/0266-3538(86)90002-3	journal	January 1986
Delamination of Composite Materials O'Brien, T. Kevin Fatigue of Composite Materials https://doi.org/10.1016/B978-0-444-70507-5.50009-3	book	January 1991
The effects of moisture and temperature on the interlaminar delamination toughness of a carbon/epoxy composite Asp, L. E. Composites Science and Technology, Vol. 58, Issue 6 https://doi.org/10.1016/S0266-3538(97)00222-4	journal	January 1998
The COMPASS force field: parameterization and validation for phosphazenes Sun, H.; Ren, P.; Fried, J. R. Computational and Theoretical Polymer Science, Vol. 8, Issue 1-2 https://doi.org/10.1016/S1089-3156(98)00042-7	journal	January 1998
A molecular dynamics study of water transport inside an epoxy polymer matrix Pandiyan, Sudharsan; Krajniak, Jakub; Samaey, Giovanni Computational Materials Science, Vol. 106 https://doi.org/10.1016/j.commatsci.2015.04.032	journal	August 2015
Molecular dynamics and micromechanics study of hygroelastic behavior in graphene oxide-epoxy nanocomposites Yang, Seunghwa; Kwon, Sunyong; Lee, Man Young Composites Part B: Engineering, Vol. 164 https://doi.org/10.1016/j.compositesb.2019.01.059	journal	May 2019
Epoxy resin thermo-mechanics and failure modes: Effects of cure and cross-linker length Chowdhury, Sanjib C.; Elder, Robert M.; Sirk, Timothy W. Composites Part B: Engineering, Vol. 186 https://doi.org/10.1016/j.compositesb.2020.107814	journal	April 2020
Prediction of quasistatic constitutive equations of moisture-absorbed epoxy polymers using atomistic simulations Park, Hyungbum; Yang, Seunghwa; Han, Jangwoo Extreme Mechanics Letters, Vol. 41 https://doi.org/10.1016/j.eml.2020.100983	journal	November 2020
Potential applications of nanotechnology in transportation: A review Mathew, Jinu; Joy, Josny; George, Soney C. Journal of King Saud University - Science, Vol. 31, Issue 4 https://doi.org/10.1016/j.jksus.2018.03.015	journal	October 2019
Structure and swelling behaviour of epoxy networks based on α,ω-diamino terminated poly(oxypropylene)-block-poly(oxyethylene)-block-poly(oxypropylene) Krakovský, Ivan; Hanuš, Jan; Pleštil, Josef Polymer, Vol. 46, Issue 1 https://doi.org/10.1016/j.polymer.2004.10.073	journal	January 2005
Moisture sorption–desorption–resorption characteristics and its effect on the mechanical behavior of the epoxy system Lin, Y. C.; Chen, Xu Polymer, Vol. 46, Issue 25 https://doi.org/10.1016/j.polymer.2005.10.002	journal	November 2005
Structure and swelling behaviour of hydrophilic epoxy networks investigated by SANS Krakovský, Ivan; Pleštil, Josef; Almásy, László Polymer, Vol. 47, Issue 1 https://doi.org/10.1016/j.polymer.2005.11.021	journal	January 2006
Molecular modeling of crosslinked epoxy polymers: The effect of crosslink density on thermomechanical properties Bandyopadhyay, Ananyo; Valavala, Pavan K.; Clancy, Thomas C. Polymer, Vol. 52, Issue 11 https://doi.org/10.1016/j.polymer.2011.03.052	journal	May 2011
A study of thermo-mechanical properties of the cross-linked epoxy: An atomistic simulation Masoumi, S.; Arab, B.; Valipour, H. Polymer, Vol. 70 https://doi.org/10.1016/j.polymer.2015.06.038	journal	July 2015
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
Moisture-Induced Reduction of Adhesion Strength between Surface Oxidized Al and Epoxy Resin: Dynamics Simulation with Electronic Structure Calculation Ogata, Shuji; Takahashi, Yusuke The Journal of Physical Chemistry C, Vol. 120, Issue 25 https://doi.org/10.1021/acs.jpcc.6b04754	journal	June 2016
Unveiling the Chemical Reactions Involved in Moisture-Induced Weakening of Adhesion between Aluminum and Epoxy Resin Ogata, Shuji; Uranagase, Masayuki The Journal of Physical Chemistry C, Vol. 122, Issue 31 https://doi.org/10.1021/acs.jpcc.8b03549	journal	July 2018
Infrared and Raman Spectra of Polyatomic Molecules. Herzberg, Gerhard; Crawford, Bryce L. The Journal of Physical Chemistry, Vol. 50, Issue 3 https://doi.org/10.1021/j150447a021	journal	March 1946
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
Structure and Dynamics of the TIP3P, SPC, and SPC/E Water Models at 298 K Mark, Pekka; Nilsson, Lennart The Journal of Physical Chemistry A, Vol. 105, Issue 43 https://doi.org/10.1021/jp003020w	journal	November 2001
Atomistic Simulation of Nafion Membrane: I. Effect of Hydration on Membrane Nanostructure Devanathan, R.; Venkatnathan, A.; Dupuis, M. The Journal of Physical Chemistry B, Vol. 111, Issue 28 https://doi.org/10.1021/jp0726992	journal	July 2007
Calibration and Testing of a Water Model for Simulation of the Molecular Dynamics of Proteins and Nucleic Acids in Solution Levitt, Michael; Hirshberg, Miriam; Sharon, Ruth The Journal of Physical Chemistry B, Vol. 101, Issue 25 https://doi.org/10.1021/jp964020s	journal	June 1997
Dielectric, Mechanical and Structural, and Water Absorption Properties of a Thermoplastic-Modified Epoxy Resin: Poly(ether sulfone)−Amine Cured Epoxy Resin Pethrick, Richard A.; Hollins, Elisabeth A.; McEwan, Iain Macromolecules, Vol. 29, Issue 15 https://doi.org/10.1021/ma9518464	journal	January 1996
Occurrence of the potent mutagens 2- nitrobenzanthrone and 3-nitrobenzanthrone in fine airborne particles Santos, Aldenor G.; da Rocha, Gisele O.; de Andrade, Jailson B. Scientific Reports, Vol. 9, Issue 1 https://doi.org/10.1038/s41598-018-37186-2	journal	January 2019
Introduction to Materials Studio Meunier, M. EPJ Web of Conferences, Vol. 30 https://doi.org/10.1051/epjconf/20123004001	journal	January 2012
Canonical sampling through velocity rescaling Bussi, Giovanni; Donadio, Davide; Parrinello, Michele The Journal of Chemical Physics, Vol. 126, Issue 1 https://doi.org/10.1063/1.2408420	journal	January 2007
A computer simulation method for the calculation of equilibrium constants for the formation of physical clusters of molecules: Application to small water clusters Swope, William C.; Andersen, Hans C.; Berens, Peter H. The Journal of Chemical Physics, Vol. 76, Issue 1 https://doi.org/10.1063/1.442716	journal	January 1982
A unified formulation of the constant temperature molecular dynamics methods Nosé, Shuichi The Journal of Chemical Physics, Vol. 81, Issue 1 https://doi.org/10.1063/1.447334	journal	July 1984
Overtone spectra of C–H bonds and vibrational a b i n i t i o study of methoxy boranes Manzanares I., Carlos; Walla, Dalat; Seburg, Randal The Journal of Chemical Physics, Vol. 95, Issue 5 https://doi.org/10.1063/1.460910	journal	September 1991
Super-stretchable metallic interconnects on polymer with a linear strain of up to 100% Arafat, Yeasir; Dutta, Indranath; Panat, Rahul Applied Physics Letters, Vol. 107, Issue 8 https://doi.org/10.1063/1.4929605	journal	August 2015
On the deformation mechanisms and electrical behavior of highly stretchable metallic interconnects on elastomer substrates Arafat, Yeasir; Dutta, Indranath; Panat, Rahul Journal of Applied Physics, Vol. 120, Issue 11 https://doi.org/10.1063/1.4962453	journal	September 2016
Canonical dynamics: Equilibrium phase-space distributions Hoover, William G. Physical Review A, Vol. 31, Issue 3 https://doi.org/10.1103/PhysRevA.31.1695	journal	March 1985
Ab initiomolecular dynamics for liquid metals Kresse, G.; Hafner, J. Physical Review B, Vol. 47, Issue 1, p. 558-561 https://doi.org/10.1103/PhysRevB.47.558	journal	January 1993
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium Kresse, G.; Hafner, J. Physical Review B, Vol. 49, Issue 20, p. 14251-14269 https://doi.org/10.1103/PhysRevB.49.14251	journal	May 1994
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
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
A model for moisture induced corrosion failures in microelectronic packages Pecht, M. IEEE Transactions on Components, Hybrids, and Manufacturing Technology, Vol. 13, Issue 2 https://doi.org/10.1109/33.56172	journal	June 1990
Molecular dynamics approach to structure-property correlation in epoxy resins for thermo-mechanical lifetime modeling Wunderle, B.; Dermitzaki, E.; Holck, O. 2009 59th Electronic Components and Technology Conference https://doi.org/10.1109/ECTC.2009.5074196	conference	May 2009
Halloysite nanotube reinforcement endows ameliorated fracture resistance of seawater aged basalt/epoxy composites Ulus, Hasan; Kaybal, Halil Burak; Eskizeybek, Volkan Journal of Composite Materials, Vol. 54, Issue 20 https://doi.org/10.1177/0021998320902821	journal	February 2020
Introduction to Epoxy Resins May, Clayton A. Epoxy Resins https://doi.org/10.1201/9780203756713-1	book	January 2018
Near-Infrared Combination and Overtone Bands of the CH₂ Sequence in CH₂X₂, CH₂XCHX₂, and CH₃(CH₂)₅CH₃ and Their Characteristic Frequency Zones Iwamoto, Reikichi; Nara, Akishi; Matsuda, Toshihiko Applied Spectroscopy, Vol. 60, Issue 4 https://doi.org/10.1366/000370206776593627	journal	April 2006
A review on the development and properties of continuous fiber/epoxy/aluminum hybrid composites for aircraft structures Botelho, Edson Cocchieri; Silva, Rogério Almeida; Pardini, Luiz Cláudio Materials Research, Vol. 9, Issue 3 https://doi.org/10.1590/S1516-14392006000300002	journal	September 2006
A Comprehensive Review on Water Diffusion in Polymers Focusing on the Polymer–Metal Interface Combination Yang, Chao; Xing, Xiao; Li, Zili Polymers, Vol. 12, Issue 1 https://doi.org/10.3390/polym12010138	journal	January 2020
Durability of an Epoxy Resin and Its Carbon Fiber- Reinforced Polymer Composite upon Immersion in Water, Acidic, and Alkaline Solutions Uthaman, Arya; Xian, Guijun; Thomas, Sabu Polymers, Vol. 12, Issue 3 https://doi.org/10.3390/polym12030614	journal	March 2020
Natural Climatic Aging of Epoxy Polymers Taking into Account the Seasonality Impact Nizin, Dmitrii R.; Nizina, T. A.; Selyaev, V. P. Key Engineering Materials, Vol. 799 https://doi.org/10.4028/www.scientific.net/KEM.799.159	journal	April 2019

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epoxy-adhesive
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molecular dynamics
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Title: Molecular Dynamics Simulation of Hygroscopic Aging Effects in Epoxy Polymer

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