The role of flow‐induced microstructure in rheological behavior and nonisothermal crystallization kinetics of polyethylene/organoclay nanocomposites

The evolution of polyethylene/organoclay nanocomposite microstructure via shear and extentional flow fields was studied by tracing rheological behavior and nonisothermal crystallization kinetics. Although studying microstructure formed through flow fields, two phenomena were noticed: the breaking of three‐dimensional (3D) network containing filler–filler, filler–matrix, and matrix–matrix interactions, and organoclay platelets orientation. Utilizing nonlinear viscoelastic measurements and thermal analyses, it was proven that clay alignment was present only in large enough shear flows and all elongational flows. It was observed that regardless of the type of flow field and its magnitude, due to the breaking of 3D network, the extent of crystallization can be increased. The half‐lives of the crystallization of film samples and those samples subjected to large enough shear rates for clay platelets to be aligned decreased, proving the effect of clay orientation on crystallization rate increment. Based on endotherms observed through melting behavior studies of samples, it was proven that in elongation and large amplitude shear flows, clay orientation had resulted in forming thicker crystalline lamellae, likely because of forcing the adjacent polymer chains to align with the clay platelets. POLYM. ENG. SCI., 54:1839–1847, 2014. © 2013 Society of Plastics Engineers