Abstract
The phase separation mechanism during the cure reaction of a liquid rubber-modified epoxy resin was investigated by light scattering, light microscopy, torsional braid analysis, electron microscopy, and differential scanning calorimetry. The binary mixture of epoxy oligomer (diglycidyl ether of bisphenol A) and carboxyl-terminated butadiene-acrylonitrile copolymer (liquid rubber) exhibited the upper critical solution temperature-type phase behaviour. The mixture loaded with curing agent was a single-phase system in the early stage of curing. When the cure reaction proceeded, phase separation took place via the spinodal decomposition induced by the increase in the molecular weight of epoxy. This was supported by the characteristic change of light scattering profile with curing time. Electron microscopy revealed that, in cured resin, the spherical rubber domains are dispersed somewhat regularly in an epoxy matrix. The regular domain arrangement seems to result from a specific situation; the competitive progress of the spinodal decomposition and polymerization; i.e. the coarsening process to irregular domain structure seems to be suppressed by network formation in the epoxy phase. It was also shown that curing at higher temperatures resulted in the suppression at an earlier stage of spinodal decomposition, and hence, shorter interdomain spacing.
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