In-rubber properties of vulcanizates deteriorate in the presence of incorporated recycled ground rubber (GR). This behavior is partly explained by a possible diffusion of sulfur from the rubber matrix into the GR. Therefore, the sulfur concentration and, thus, the crosslink density in the matrix are reduced. This phenomenon was further investigated in this research work using two spatially resolved methods that supplement each other: the diffusion of soluble sulfur in GR-containing compounds was locally investigated via Micro X-Ray Fluorescence analysis. Viscoelastic properties were also determined spatially by the Micro Dynamic-Mechanical Indentation method. Combining the results of both methods, local concentrations of sulfur were related to local viscoelastic properties, revealing great differences in crosslink density at the interface between the GR and matrix material. In this way, it is shown that sulfur is capable of diffusing several mm, which locally doubles its concentration with respect to the sulfur content of the compound formulation. This, in turn, negatively impacts the homogeneity of crosslink density in both the matrix and GR, revealing a local increase in the elastic stiffness of 100 %. In addition, it was found that the vulcanization characteristics of the used polymers determine the amount of sulfur diffusion and, thus, the change in viscoelastic properties.
Keywords: crosslink density; ground rubber; indentation; recycling; sulfur diffusion; viscoelasticity; x-ray fluorescence.