Bound rubber in elastomers: Analysis of elastomer‐filler interaction and its effect on viscosity and modulus of composite systems

Abstract Bound rubber measurement may be very misleading as a measure of elastomer–carbon black interaction because sometimes only part of the apparently bound rubber is truly adsorbed on the carbon black surface. A theory is proposed which utilizes bound rubber measurements, but separates truly adsorbed rubber from other insoluble gel and enables calculation of the adsorbed elastomer layer thickness, a numerical value of interaction. Measurements of interaction were obtained for many different rubbers, including polybutadienes, styrene–butadienes, EPDMs, and butyl, with several different furnace blacks. An equation for viscosity of a rubber–carbon black composite is proposed, based on the degree of interaction obtained from the theory and the possible varying degree of orientation of the composite as the rate of shear is changed. This has been applied experimentally both to soluble elastomers and to an elastomer containing a nonrigid gel. The modulus of a vulcanized composite is shown to be related to the effective volume fraction of filler, which is equivalent to the volume fraction of filler plus adsorbed rubber, at temperatures above the glass transition temperature, regardless of the type of rigid filler. Below the glass transition temperature, the modulus depends only on the filler volume concentration.