Nonlinear viscoelastic behavior and their time-temperature superposition for filled styrene butadiene rubber compounds and vulcanizates

The nonlinear viscoelastic behavior of rubber composites is of great practical importance in their processing as well as the application. In this paper, nonlinear viscoelastic behavior for vulcanized and unvulcanized filled styrene butadiene rubbers (SBR), SBR/carbon black (CB) composites, were mainly investigated. Besides the conventional Payne effect, frequency (ω) sweep tests at different strains (linear and nonlinear viscoelastic regions) were performed to get more information about viscoelastic response, especially in nonlinear region that close to actual driving conditions. Conductivity synchronization test was also operated to explore the evolution of CB agglomerates. It reveals that the filler network structure recovers slowly but the rubber network recovers rapidly during an increasing and decreasing strain sweep cycle. At large strain, rheological parameters of vulcanizates change significantly with increasing ω. A pseudomaster curve based on the ω sweep at large strain and different temperature can be obtained both for compounds and vulcanizates, indicating that the time-temperature superposition is also applicable to the nonlinear viscoelastic behavior. Similar linear and nonlinear viscoelastic behaviors of filled vulcanizates to that of unfilled vulcanizates demonstrate the same mechanism of viscoelastic response. The loss modulus peak of filled vulcanizates primarily comes from the Rouse movement of rubber chains between crosslinking points. Under large strain, the strain amplication effect of particles hardly influence the characteristic relaxation time of Rouse movement between crosslinking points.