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The antagonistic effect of processing and thermal annealing on both thefiller structure and the polymer matrix is explored in polymer nanocompositesbased on natural rubber with precipitated silica incorporated by coagulationfrom aqueous suspension followed by roll-milling. Their structure and linearand non-linear rheology have been studied, with a particular emphasis on theeffect of high temperature thermal treatment and the number of milling passes.Small-angle X-ray scattering intensities show that the silica is organized insmall, unbreakable aggregates containing ca. 50 primary nanoparticles, whichare reorganized on a larger scale in filler networks percolating at the highestsilica contents. As expected, the filler network structure is found to besensitive to milling, more milling inducing rupture, as evidenced by thedecreasing Payne effect. After thermal treatment, the nanocomposite structureis found to be rejuvenated, erasing the effect of the previous milling on thelow-strain modulus. In parallel, the dynamics of the samples described by therheology or the calorimetric glass-transition temperature remain unchanged,whereas the natural latex polymer network structure is modified by millingtowards a more fluid-like rheology, and cannot be recovered.

Rejuvenating the structure and rheological properties of silica nanocomposites based on natural rubber