Aggregation of fillers blended into random elastomeric networks: theory and comparison with experiments

Abstract

A theoretical model describing aggregation of filler particles in amorphous elastomers is proposed. The model is based on a counting technique originally used in genome analysis to characterize the size and distribution of overlapping segments randomly placed on a DNA molecule. In the present model, the particles are first assumed to aggregate randomly upon mixing into the elastomer and their sizes are calculated. The sizes and distributions of aggregates are also studied in the presence of attractive interparticle forces. Results of the proposed model are compared with experimental data on silica-filled end-linked poly(dimethylsiloxane) networks. Comparison of the theory and experiment shows that the random aggregation assumption where no attractive forces exist between the particles is not valid and a significant attraction between the silica particles is needed in the theory to justify the experimental data obtained using atomic force microscopy. For filler content below 1.45 vol.%, the model agrees, qualitatively, with experiment and shows the increase in cluster size with increasing amount of filler. It also explains the increase in the dispersion of aggregate sizes with increasing amount of filler.