A high-temperature dielectric process as a probe of large-scale silica filler structure in simplified industrial nanocomposites.

The existence of two independent filler-dependent high-temperature Maxwell-Wagner-Sillars (MWS) dielectric processes is demonstrated and characterized in detail in silica-filled styrene-butadiene (SB) industrial nanocomposites of simplified composition using Broadband Dielectric Spectroscopy (BDS). The uncrosslinked samples are made with 140 kg mol(-1) SB-chains, half of which carry a single graftable end-function (50% D3), and Zeosil 1165 MP silica incorporated by solid-phase mixing. While one high-temperature process is known to exist in other systems, the dielectric properties of a new silica-related process - strength, relaxation time, and activation energy - have been evidenced and described as a function of silica volume fraction and temperature. In particular, it is shown that its strength follows a percolation behavior as observed with the ionic conductivity and rheology. Moreover, activation energies show the role of polymer layers separating aggregates even when they are percolated. Apart from simultaneous characterization over a broad frequency range up to local polymer and silanol dynamics, it is believed that such high-temperature BDS-measurements can thus be used to detect reorganizations in structurally-complex silica nanocomposites. Moreover, they should contribute to a better identification of dynamical processes via the described sensitivity to structure in such systems.