AbstractThe temperature dependence of the dynamic viscoelastic behavior of interpenetrating networks (IPN) of polyurethane (PU) prepared from poly(oxypropylenediol) (POP) and toluylene diisocyanate (TDI), and of polyurethane diacrylate (PUA) prepared from POP and TDI by reacting isocyanate groups of the prepolymer with 2‐hydroxyethyl acrylate, was measured in the main transition region. The photoelastic behavior of IPN swollen in dimethylformamide (DMF) and methyl ethyl ketone (MEK) was examined in the rubbery region. The temperature dependences of the dynamic Young modulusE*of IPN in the concentration range of PUA ≥ 50 vol. indicate a pronounced two‐phase behavior. The effect of the composition of IPN on the temperature dependence of the modulusE*was quantitatively described by Takayanagi's two‐phase model with the conclusion that the PU network is the continuous phase of IPN at ≤ 90 PUA. While in the range of high concentrations of PUA (≥50) the contributions of phases toE*are additive within the whole range of temperatures, the thermomechanical behavior at low PUA concentrations (≤40) is more complex. This finding is interpreted by the existence of an interfacial layer which leads to the loss of the distinct two‐phase character of IPN. The higher number of elastically active network chains (EANC) of the PUA network compared with the PU network corresponds to different molecular weights of POP used in the preparation of both components. The nonadditive dependence both of the concentration of EANC and of the stress‐optical coefficient on composition confirms the heterogeneous character of
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