Stress-induced interfacial failure in filled polymer melts

We study a dynamic interfacial slip phenomenon in filled polymer melts. When a poly(dimethyl siloxane) melt of weight average molecular weight M_w = 93 700 is mixed with glass beads of diameter up to 45 m, the sample shows some evidence of breakdown of interfacial adhesion between the glass beads and the PDMS matrix at a level of oscillatory stress under which the pure PDMS melt exhibits no decay. The decay of viscoelastic properties with time is essentially independent of the amplitude of shear strain as long as the magnitude of the oscillating stress is sufficiently high. It is suggested that much higher local stress than the apparent applied stress may be generated between the narrowly spaced beads. The interfacial slip was observable because it was measured against a natural length scale d in the filled polymer melts which is the filler size or the inter-filler distance and is much smaller than the dimensions of the flow cell. The decay under high stress and healing of interfacial adhesion upon a large reduction in stress may be related to the de-bonding and reformation of hydrogen bonds between the PDMS chains and the glass bead surfaces.