Abstract
A large body of experimental work on the microstructure and dynamics of simplifiedindustrial nanocomposites made of disordered silica filler in a styrene-butadiene matrixby solid-phase mixing is regrouped and critically discussed in this feature article. Recentresults encompass systems with varying polymer mass, grafting functionality, and fillercontent. They have been obtained by simulation-based structural modelling of nanoparticleaggregate size and mass deduced from small-angle scattering and transmission electronmicroscopy. Our model has been validated by independent swelling experiments.Comparison of structurally-close nanocomposites of widely different chain mass led tothe identification of a unique structure-determining parameter, the grafting density, aswell as to a unified picture of aggregate formation mechanisms in complex nanocompositesduring mixing. In addition, low-field proton NMR allowed for the characterization ofdynamically slowed-down (‘glassy’) polymer layers, which were shown not to dominatethe rheological response, unlike the structural contribution. Finally, broadband dielectricspectroscopy was used in an innovative manner to identify filler percolation – also identifiedby rheology – via dynamics along filler surfaces.