A new class of epoxy nanocomposites with completely defined organic/inorgan
ic phases was prepared by reacting octakis(glycidyldimethylsiloxy)octasilse
squioxane [(glydicylMe(2)SiOSiO(1.5))(8)] (OG) with diamino-diphenylmethane
(DDM) at various compositional ratios. The effects of reaction curing cond
itions on nanostructural organization and mechanical properties were explor
ed. A commercial epoxy resin based on the diglycidyl ether of bisphenol A (
DGEBA) was used as a reference material throughout these studies. FTIR was
used to follow the curing process and to demonstrate that the silsesquioxan
e structure is preserved during processing. OG/DDM composites possess compa
rable tensile moduli (E) and fracture toughness (KIC) to, and better therma
l stabilities than, DGEBA/DDM cured under similar conditions. Dynamic mecha
nical analysis and model reaction studies suggest that the maximum cross-li
nk density is obtained at N = 0.5 (NH2:epoxy groups = 0.5) whereas the mech
anical properties are maximized at N = 1.0. Digestion of the inorganic core
with HF followed by GPC analysis of the resulting organic tether fragments
when combined with the model reaction studies confirms that, at N = 0.5, e
ach organic tether connects four cubes, while, at N = 1.0, linear tethers c
onnecting two cubes dominate the network structure. Thus, well-defined nano
composites with controlled variation of the organic tether architecture can
be made and their properties assessed.