Restricted dynamics in polymer-filler systems

Composites in which fibres or fillers are incorporated into a polymeric component exhibit improved mechanical strength compared to the polymer matrix. This reinforcement effect strongly depends on the properties of the interphase and the specific interactions between the polymer and the reinforcing additive. A wide range of experimental methods have been used to assess the effect of active fillers on the mobility of the polymer chains. The experimental results from NMR, dielectric spectroscopy and dynamical thermal analysis reveal that the mobility of chain units adjacent to the adsorbed surface differs considerably from the bulk. We have used quasielastic neutron scattering to investigate the dynamic properties of poly(dimethyl siloxane) (PDMS) filled with silica particles. This technique which probes the motion of the hydrogen atoms has been extensively used to study the local dynamics of polymeric materials. In this paper we show that QENS provides detailed information on the reduced mobility of chain segments in polymer-filler systems. QENS measurements were carded out on PDMS filled with hydrophilic Aerosil with different specific surface area (average diameter 7 and 20 nm). Detailed data analysis indicates that the QENS spectra of the polymer-filler composites can be described by the sum of two contributions: (a) a quasielastic component due to chains not affected by the presence of the fillers and (b) an elastic term from those chain segments strongly affected by the presence of fillers. The latter depends on the specific surface area of the particles and their weight fraction in the composite.