Peculiarities in the structure - properties relationship of epoxy-silica hybrids with highly organic siloxane domains

Epoxy-silica hybrids were produced from a diglycidyl ether of bisphenol-A resin using Jeffamine 230 hardener with a two-step in situ generation of siloxane domains. The siloxane component was obtained by hydrolysis and condensation of a mixture of γ-glycidoxypropyl-trimethoxysilane and tetraethoxysilane, which was added to the epoxy resin after removal of the formed alcohols and water. The morphological structure of the hybrids was examined by TEM, SAXS and WAXS analysis, and confirmation of the identified co-continuity of the constitutive phases for nominal silica contents greater than 18%wt was obtained by TGA and DMA analysis. While the loss modulus was found to increase monotonically over the entire range of siloxane content, the glass transition temperature exhibited a stepwise increase upon reaching the conditions for phase co-continuity. Molecular dynamics simulations were used to produce model structures for silsequioxanes cage-like structures, as main constituents of the siloxane phase. The predicted interdomain distance between the silsequioxane structures was in agreement with the SAXS experimental data.