Filled rubbers were prepared using radical polymerization. Colloids used are monodisperse and spherical, their surface is functionalized with silane creating covalent bonding or inert to the polymer. We have shown that the dispersion state obtain for these two kind of silanes were similar using Small Angle Neutron Scattering and cryo-TTEm imaging. The so formed network was studied by 1H NMR, swelling ratio at equilibrium to determine the kind of interaction at the interface (covalent, hydrogen, van der Waals). We shown that interaction were of two types: covalent and hydrogen for our systems. NMR also allows us to determine the quantity of immobilized polymer at the interface. This glassy layer is situated around silica particles. This studied shows that the glassy layer is strongly related to the number of silane at the interface, to the interaction type, to the temperature and to the distance between fillers. Viscoelastic properties of these elastomers were measured at low strain. Properties are strongly related to the existence of this galssy layer and its dependence in term of distance between fillers and temperature. We have also seen a new frequency behavior of non-covalent interacting systems. At medium deformation (Payne regim) we show the existence of at least two types of non-linearity. First one is associated to the glassy layer through its plastization under strain. The second is still not yet understaood, but is associated with the breakage of hydrogen bonding and to some extend at a particular dynamic at the interface.
