Molecular dynamics simulations of EPON-862/DETDA epoxy networks: structure, topology, elastic constants, and local dynamics

SV Kallivokas and AP Sgouros and DN Theodorou, SOFT MATTER, 15, 721-733 (2019).

DOI: 10.1039/c8sm02071j

Structural, topological, mechanical and dynamical properties of EPON-862/DETDA epoxy networks are investigated with Molecular Dynamics (MD) simulations. The epoxy networks are composed of the resin Diglycidyl Ether Bisphenol F (DGEBF), also known as EPON-862, and the hardener Diethyl Toluene Diamine (DETDA). Systems with four different crosslinking degrees are examined; the effect of the degree of crosslinking on studied properties is thus determined. The computed quantities are retrieved by employing several simulation strategies and numerical methods of statistical mechanics in order to gain a rigorous and solid understanding of the aforementioned properties as well as to assess the accuracy and applicability of the methods employed. We quantify and analyze the local structure of the EPON-862/DETDA epoxy networks through the partial pair distribution functions, the Faber- Ziman partial structure factors and through simulated X-ray diffraction patterns, demonstrating good agreement with an experimental spectrum from a similar epoxy resin. The topology of the networks is examined with the aim of assessing percolation of connectivity, the properties of network fragments (subnetworks), and the distribution of functionalities of the crosslinks. The elastic constants of the systems are retrieved by employing two equilibrium (analysis of volume fluctuations, Parrinello- Rahman strain fluctuation relation) and one nonequilibrium (uniaxial tension/compression deformations at prescribed rate) method. Finally, the glass temperatures of the systems are estimated by calculating the density as a function of temperature and by analyzing the reorientational dynamics of bond vectors which describe relaxation processes at the segment level.

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