Co-Extrusion Layer Multiplication of Rheologically Mismatched Polymers: A Novel Processing Route

Co-extruded films with up to 65 layers of two rheologically mismatched polymer systems - polystyrene/poly(methylmethacrylate) (PS/PMMA) and hard/soft thermoplastic polyurethanes (TPUs) - were successfully produced using a combination of a 9-layer feedblock, low-pressure drop multiplier dies, and external lubricants. Formation of viscoelastic instabilities was studied using a custom visualization and by finite element method (FEM) simulations of a standard multiplier. The results showed that the flow inside the standard multiplier die is highly non-uniform, with severe gradients in shear and normal stresses and viscous encapsulation occurring mainly in the initial multiplication stages where there is enough material available in the low-viscosity layers to proceed with the encapsulation. To mitigate layer degradation the standard 2- or 3-layer feedblock was replaced with a 9-layer one, thereby decreasing the thickness of each layer at the end of the feedblock. Also, subsequent layering was performed using a low flow resistance die. This new multiplier die yields a more uniform flow profile and imparts a more homogeneous thermo-mechanical history on the melt which results in an improved layer stability. Simulations showed that in the standard die the second normal-stress difference (N-2) responsible for elastic instabilities at the edges of the die are very high. These can be reduced by inducing slip at the wall resulting in be much improved layer uniformity and stability. This was accomplished experimentally via the use of external lubricants, and the resulting layered structure was indeed much better than was possible to achieve with the conventional multiplier dies.