During the “slit die extrusion-hot stretching” process, highly oriented polyamide 6 (PA6) dispersed phase was produced and retained in the polypropylene (PP) matrix directly. By adjusting the stretching forces, the PA6 spherical phase evolved into the ellipsoid, rod-like microfibril with a decreasing average diameter; then, the PA6 microfibrils broke. Moreover, the effects of the PA6 phases formed in the process of the microfibrillation on PP’s crystallization behaviors were studied systematically. As the stretching forces increased, the crystallization ability and orientation degree of PP crystals improved significantly. Differential scanning calorimetry and polarizing optical microscopy confirmed the formation of PP spherulite, fan-shaped lamellae and a transcrystalline layer under the induction of the PA6 phases with different morphology. In the PP/PA6 microfibrilar composites (MFCs), PP crystals showed smaller average size, more crystals and stronger interface adhesion due to more excellent heterogeneous nucleation ability of the PA6 microfibrils, which made contributions to the improvement of the melt elasticity responses and oxygen barrier properties of the PP/PA6 polymer blends.
The microstructure evolution of an isotactic polypropylene (iPP) sheet during solid-state stretching was studied. The transition of the spherulites—cylindrites was evaluated using in-situ two-dimensional wide-angle and small-angle X-ray scattering methods. The crystallinity of stretched iPP sheets was characterized by differential scanning calorimetry. The crystal morphology was observed by means of scanning electron microscopy. It was found that the differences of crystal microstructure of the iPP sheet depended on the stretching strain, which promoted the orientation of molecular chains. Amorphous molecular chains in the spherulites oriented and formed into a mesophase near the yield point, and the partially ordered mesophase was further stretched to form an oriented cylindrite structure after the yield point. The highest relative content of cylindrites appeared at 15% strain. Notably, as the amorphous phase embedded into the lamellae layer, the crystal size decreased with the increase of strain, which indicated that the crystallinity of the stretched iPP sheet was much higher than that of unstretched iPP sheet. The induced cylindrites structure played a more important role in improving the mechanical properties and heat resistance of iPP sheets. Compared with the unstretched iPP sheets, the tensile strength increased by 28%, the notch impact toughness significantly increased by 78%, and the vicat softening point increased from 104 to 112 °C.
The deformation-induced crystallization of an isotactic polypropylene (iPP) sheet containing a β-nucleating agent was evaluated. The phase transformation of the β-modifications was investigated and the crystal morphology was observed at room temperature after stretching at different temperatures. The results showed that the crystallinity increased after solid-state stretching. When the stretching temperature was below the initial crystallization temperature, stretching deformation promoted the orientation of amorphous molecular chains. When the deformation temperature exceeded the crystallization temperature, part of the β-modifications underwent a phase transformation process and was stretched into a shish-kebab structure. However, once the stretching temperature was close to the melting point, the β-modifications melted and recrystallized, and the shish-kebab structure underwent stress relaxation due to poor thermal stability, transforming into α-modifications. It was revealed that the crystal phase transformation mechanism of the β-modifications was based on the orientation of the molecular chains between the adjacent lamellae. In addition, the shish-kebab cylindrite structure played an important role in modifying the tensile and impact properties of the iPP sheet. The tensile and impact strengths increased by as much as 34% and 126%, respectively.
In this work, carbon black (CB)/polyamide 6 (PA6)/polypropylene (PP) microfibrillar composites (MFCs) were fabricated through an extrusion (hot stretching) heat treatment process. The CB-coated conductive PA6 microfibrils with high aspect ratio were in situ generated as a result of the selective accumulation of CB at the interface. At the proper temperature, a 3D entangled conductive structure was constructed in the PP matrix, due to topological entanglement between these conductive microfibrils. This unique conductive structure provided the PP composites with a low electrical conductivity percolation threshold. Moreover, the electromechanical properties of conductive MFCs were investigated for the first time. A great stability, a high sensitivity and a nice reproducibility were achieved simultaneously for CB/PA6/PP MFCs. This work provides a universal and low-cost method for the conductive polymer composites’ (CPCs) fabrication as sensing materials.
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