Molecular dynamics study on the influence of thermal aging on the mechanical properties of epoxy resins for high...

Thermal aging significantly deteriorates the mechanical properties and service performance of epoxy resins used for the high-voltage bushing. Current studies on the thermal aging behavior of epoxy resins mainly focus on experimental observations. However, an in-depth understanding of the mechanism of thermal aging of epoxy resins requires the monitoring of structural evolution of epoxy resins during thermal aging at the molecular level. To thoroughly analyze the intrinsic factors affecting structural evolution and the effect of thermal aging on the mechanical properties of epoxy resin for high-voltage bushing, epoxy resin models with different crosslinking degrees were established and thermal aging treatments at various temperatures and time periods were carried out by molecular dynamics simulation. It was found that the tensile strength of the epoxy resin was enhanced with the increase of the crosslinking degree, which was related to the elevation of the proportion of C-N and O-H bonds in its structure. With the increase of thermal aging temperature, the tensile strength of the epoxy resin decreased, which was related to the formation of weak bonds. At the early stage of thermal aging and after a period of high-temperature thermal aging, the strength of epoxy resin significantly decreases. The thermal aging of the epoxy resin is accelerated under external loading. In addition, the crosslinking degree and curing agent also affect the thermal aging resistance of epoxy resins. The results of this study can provide guidance for predicting and improving the thermal aging resistance of epoxy resins.

Materials Studio was used to construct molecular models and complete crosslinking reactions. DGEBA and 44DDS (or 33DDS) were mixed at a ratio of 2:1, followed by crosslinking reaction. During this process, the Nose method was used to control temperature, the Berendsen method was used to control pressure, and the polymer consistent force field (PCFF) was used to control the motion and force of atoms. Isobaric-isothermal ensemble (NPT ensemble) was used to heat up epoxy resin models to various thermal aging temperatures of 400 K, 500 K, 600 K and 700 K. The models were maintained at these temperatures for different thermal aging times of 100 ps, 200 ps, 300 ps, 400 ps, 500 ps, 600 ps, 700 ps and 800 ps. Afterwards, the models were cooled down to 300 K and subjected to uniaxial tensile testing at this temperature with a strain rate of 1 × 10⁹ s^-1. The structural configurations and stress-strain data during the tensile process were recorded. The flow stress of the material was derived by counting the average stress in the 20-50% strain interval.