Reinforcement mechanisms in carbon black and silica loaded rubber melts at low stresses

For a range of different fillers, silicas and carbon blacks, added to a rubber melt at various concentrations, dynamic moduli in the linear viscoelastic limit have been determined. It is shown that reinforcement is dire to hydrodynamic effects and the formation of a Secondary particulate structure within the rubber matrix. Both mechanisms can be distinguished experimentally by a frequency sweep. Hydrodynamic reinforcement depends on the filler volume to which immobilized polymer must be added. Its concentration dependence is well described by the semiempirical exponential Thomas Equation. Nominal and effective filler loadings are related by concentration-independent effectiveness factors which can be modelled for all types of fillers considering an immobilized layer of constant height around an agglomerated cluster of filler particles. This provides an explanation for the well-known dependence of reinforcement ability on surface area at small stresses. The chemical and microscopic structure of the filler surface appears to be less important with respect to immobilization ability in the linear viscoelastic regime. The secondary structure formed by the particles is found to be tied together by the elastomer. its modulus correlates with the filler's immobilization ability and shows little dependence on the filler nature. Due to formation of a filler-polymer structure with individual relaxation times, a strict separability of hydrodynamic and interparticular-reinforcement mechanisms at very high loadings no longer applies.