Rheology of SiO2/(acrylic polymer/epoxy) suspensions. II. Nonlinear stress relaxation

Large deformation, nonlinear stress relaxation modulus G(t, γ) was examined for the SiO₂ suspensions in a blend of acrylic polymer (AP) and epoxy (EP) with various SiO₂ volume fractions (?) at various temperatures (T). The AP/EP contained 70 vol.% of EP. At ??≤?30 vol.%, the SiO₂/(AP/EP) suspensions behaved as a viscoelastic liquid, and the time-strain separability, G(t, γ)?=?G(t)h(γ), was applicable at long time. The h(γ) of the suspensions was more strongly dependent on γ than that of the matrix (AP/EP). At ??=?35 vol.% and T?=?100°C, and ??≥?40 vol.%, the time-strain separability was not applicable. The suspensions exhibited a critical gel behavior at ??=?35 vol.% and T?=?100°C characterized with a power law relationship between G(t) and t; G(t)?∝?t ^???n . The relaxation exponent n was estimated to be about 0.45, which was in good agreement with the result of linear dynamic viscoelasticity reported previously. G(t, γ) also could be approximately expressed by the relation $G(t,\gamma) \propto t^{-n^{\prime}}$ at ??=?40 vol.%. The exponent n ^′ increased with increasing γ. This nonlinear stress relaxation behavior is attributable to strain-induced disruption of the network structure formed by the SiO₂ particles therein.