Abstract
In this thesis, we study nanocomposite materials made of rubber (styrene-butadien copolymer "SBR") reinforced by highly dispersible silica nanofillers. In order to identify physico-chemical mechanisms responsible for such a reinforcement and being able to optimize it, we must understand existing correlations between the material macroscopic properties and the multi-scale structure of the filler. For this purpose, a wide campaign of small angle X-ray scattering (SAXS) and electronic microscopy experiments have been performed. Coupling this data with Monte-Carlo simulations led to the emergence of a concept describing the silica morphology: A branched tridimensional network built up from aggregates (radius 50 nm) made of nanoparticles (radius 10 nm) spreading across in the whole sample. The analysis of the reinforcement in nanocomposites is based on rheometry and dynamic mechanical analysis. Other techniques like dielectric spectroscopy, nuclear magnetic resonance, thermogravimetric analysis or infra-red spectrometry contributed as well to fully characterize these materials, particularly to probe the SBR chains dynamic at the interface with the filler. In order to reveal the correlations between structure and properties, we systematically described the impact of key parameters such as filler fraction, polymer grafting or the chain molar mass on the silica morphology (aggregates size, ...) as well as on the mechanical behavior (elastic modulous, ...) of the composites. This work allowed identifying the polymer grafting density as the parameter defining the filler structure and playing a significant role on the reinforcement. This thesis, firmly focused on fundamental comprehension, contributes to the development of a general law describing the effect of the filler structure on the performance of tires. The latter must provide answers to engineering issues concerning wear resistance, wet grip or rolling resistance. Moreover, in order to obtain additional information regarding the rubber-silica interactions, we developed an experimental process allowing the production of "model" systems reinforced with colloidal silica. The use of such filler, very well defined in terms of size and shape, makes much easier the structural analysis giving the opportunity to investigate deeper the effective potential between the two phases during the composite production.