Common Origin of Filler Network Related Contributions to Reinforcement and Dissipation in Rubber Composites

A comparative study focusing on the visco–elastic properties of two series of carbon black filled composites with natural rubber (NR) and its blends with butadiene rubber (NR-BR) as matrices is reported. Strain sweeps at different temperatures are performed. Filler network-related contributions to reinforcement (ΔG′) are quantified by the classical Kraus equation while a modified Kraus equation is used to quantify different contributions to dissipation (ΔGD″, ΔGF″). Results indicate that the filler network is visco-elastic in nature and that it is causing a major part of the composite dissipation at small and intermediate strain amplitudes. The temperature dependence of filler network-related reinforcement and dissipation contributions is found to depend significantly on the rubber matrix composition. We propose that this is due to differences in the chemical composition of the glassy rubber bridges connecting filler particles since the filler network topology is seemingly not significantly influenced by the rubber matrix for a given filler content. The underlying physical picture explains effects in both dissipation and reinforcement. It predicts that these glassy rubber bridges will soften sequentially at temperatures much higher than the bulk Tg of the corresponding rubber. This is hypothetically due to rubber–filler interactions at interfaces resulting in an increased packing density in the glassy rubber related to the reduction of free volume. From a general perspective, this study provides deeper insights towards the molecular origin of reinforcement and dissipation in rubber composites.