Binder/Filler Interaction and the Nonlinear Behavior of Highly-Filled Elastomers

Abstract

Abstract 1. The small-deformation-viscoelastic response of elastomers containing nonreinforcing filler has been investigated. Nonlinear viscoelastic behavior was observed as a pronounced strain-amplitude dependence. The degree of this dependence was quantified using a power-law representation as a single nonlinear parameter, m. 2. The magnitude of m was a function of formulation variables. It was found that m increased with the volume fraction and particle size of filler material, as well as the volume fraction of plasticizer. Reduced values of m were observed in the presence of bonding agent and with greater degrees of apparent crosslinking. The latter was controlled in this study through imbalanced urethane cures. 3. Nonlinear behavior of elastomers containing nonreinforcing filler has been compared and contrasted with the data base for carbon-black-reinforced elastomers. The major difference is in the effect of the surface area of filler particles. Nonlinear response in black-filled rubbers increases with surface area, while the opposite is reported in this study. Additionally, the relationship between viscoelastic dissipation and the magnitude of nonlinear response, well established for black-filled rubbers, was not observed. These results indicate that the response of elastomers containing nonreinforcing filler, although nearly identical in appearance to that seen with reinforcing filler, is not driven by the same mechanism. 4. A binder/filler interaction model is proposed for materials containing nonreinforcing filler. This model is based on the ideal adhesive strength of the binder/filler interface. In this model, greater attraction between polymer and particle surfaces reduces molecular slippage during deformation, leading to a decreased dependence of the modulus on strain amplitude, or decreased nonlinearity. It is shown that the model provides reasonable predictions for the observed phenomena.