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Molecular Dynamics Simulation of Hygroscopic Aging Effects in Epoxy Polymer

  • Thematic Section: 6th World Congress on Integrated Computational Materials Engineering
  • Published:
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Abstract

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%. 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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Data Availability

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

This work was supported by the High-Performance Computing for Energy Innovation (HPC4EI) Initiative, managed by U.S. Department of Energy’s Office of Energy Efficiency and Renewable Energy (EERE). The project was funded by EERE Vehicle Technologies Office. Pacific Northwest National Laboratory is operated for the U.S. Department of Energy by Battelle under Contract DE-AC06-76RLO1830. This research used resources of the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under Contract No. DE-AC02-05CH11231.

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Authors and Affiliations

  1. Pacific Northwest National Laboratory, Richland, WA, 99354, USA

    M. F. N. Taufique & Ram Devanathan

  2. PPG Coatings Innovation Center, Allison Park, PA, 15101, USA

    Martin Losada, Matthew J. DiTucci, Loubna Pagnotti, Daniel Willis & Matthew Torres

  3. Physical and Life Sciences Directorate, Lawrence Livermore National Laboratory, Livermore, CA, 94550, USA

    Sebastien Hamel & Nir Goldman

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  1. M. F. N. Taufique
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  9. Ram Devanathan
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Contributions

MFNT and ML have equal contribution as first author. MFNT performed MD simulations, analyzed the results, and wrote the manuscript. ML built monomer molecular models of epoxy and curing agents, constructed the cross-linked models and performed MD simulations with different crosslinking densities. MJD performed analysis of NIR spectral data and LP, DW, and MT acquired MIR and NIR data, respectively. NG and SH performed DFT-MD calculations. RD provided technical expertise to MD simulated data, interpreted the results, and reviewed the manuscript.

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Correspondence to M. F. N. Taufique.

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Taufique, M.F.N., Losada, M., Hamel, S. et al. Molecular Dynamics Simulation of Hygroscopic Aging Effects in Epoxy Polymer. Integr Mater Manuf Innov 12, 185–195 (2023). https://doi.org/10.1007/s40192-023-00296-5

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