Understanding the Strain-Dependent Dielectric Behavior of Carbon Black Reinforced Natural Rubber: An interfacial or bulk phenomenon?

Filler-polymer interactions are one of the keys to understanding the physical properties of polymer composites. These interactions give rise to an interface with specific properties that may have a nontrivial effect on the macroscopic properties of composites. Direct measurement of the interface properties at nanometer scale is usually unavailable. Thus, interface properties are often back calculated from the bulk response using a computational model. However, if the model does not take into account the morphology of the filler dispersion, the results can be misleading. Recently it has been found that the dielectric response of a carbon black filled natural rubber film can change dramatically upon stretching [Huang, Macromolecules 49, 2339 (2016)]1. In this paper, we will show that this phenomenon can be largely explained by changes in filler cluster connectivity due to strain and is probably not caused by changes in the interfacial interactions. To support the argument, the polarization mechanism of the composites in the measured frequency range is analyzed and numerical models are developed to virtually reproduce the physical phenomenon as a function of strain. As a result, a power-law dependence of dielectric permittivity with strain is derived, which matches closely with the experimental results.