Melt rheology of nanocomposites based on acrylic copolymer and cellulose whiskers

Nanocomposites based on poly(styrene-co-hexylacrylate) copolymer and cellulose whiskers as the nano-size filler were prepared by in situ miniemulsion polymerization and their melt rheological behaviours were investigated under dynamic shear conditions. The effects of gamma-methacryloxypropyl triethoxysilane (MPS) content along with the whisker loading were explored. In the absence of whiskers, a transition from a liquid- to a solid-like behaviour was observed when the polymer was synthesized in the presence of MPS. When cellulose nanofiller was added, the storage modulus G' and the dynamic viscosities of the nanocomposites increased monotonically with whisker content and the resulting materials displayed a solid-like behaviour. Above 2 wt.%. loading, a percolated interconnected whisker-whisker network is built up, producing a jump in the storage modulus and strong shear-thinning behaviour of the viscosity. However, as the nanocomposites were prepared in the presence of 3% of MPS, no enhancement nor in the storage modulus nor in the viscosity was observed up to 5 wt.%. of whisker loading. Such a phenomenon was ascribed to inhibition of build-up of the whisker network. The non-linear viscoelastic behaviour of the nanocomposites was also investigated and analysed in terms of the breakdown of different networks, namely the filler-filler and the polymer-filler networks. (C) 2011 Elsevier Ltd. All rights reserved.