Abstract

End‐linking poly(dimethylsiloxane) was used to prepare bimodal elastomers networks so as to have inhomogeneous nanostructures, and also to prepare others having very broadly multimodal chain‐length distributions. Macroscopic phase separation, probably high crosslink density clusters, was observed to occur in some of the bimodal networks. The mechanical properties in simple extension and in equilibrium swelling were measured. The bimodal elastomers that were not obviously inhomogeneous showed very good mechanical properties, but the macroscopically phase‐separated networks, and the broadly multimodal network were weak. Analysis of the Mooney‐Rivlin profiles suggests that the reinforcing mechanism could have a structural component in addition to that from the limited extensibilities of the short chains. The mechanical properties and the extents of swelling support the cluster conjecture, in accord with previous morphological studies on spatially‐inhomogeneous polysiloxane elastomers.

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