Stress-induced microphase separation of interlamellar amorphous phase in hard-elastic isotactic polypropylene film

Abstract

Lamellar stacks, arranged alternatively with hard crystal and soft amorphous nano-layers, are the basic building units to determine the intrinsic mechanical properties of semi-crystalline polymeric materials. The mechanical instability of hard-elastic isotactic polypropylene (iPP) films with highly parallel lamellar stacks is studied with in-situ synchrotron radiation small- and wide-angle X-ray scattering (SAXS/WAXS) techniques during cyclic tensile deformation. Unexpectedly, the micro-strain, deduced from the relative variation of lamellar periodicity, shows an accelerated increase at the onset of instability and reaches values larger than the corresponding macro-strain after yield, during which no irreversible plastic destruction of crystal is observed. Combining the unpredictable increase of long period and other structural information obtained with in-situ SAXS/WAXS measurements, we propose that stress-induced microphase separation of interlamellar amorphous phase is responsible for the yield behavior and the hyperelasticity of hard-elastic iPP films, which stems from the heterogeneous distribution of tie chain/trapped entanglement in interlamellar amorphous nano-layers. This reversible stress-induced non-equilibrium phase transition of interlamellar amorphous phase is different from current plastic deformation models with crystal destruction in semi-crystalline polymers but in line with the nearly 100% elastic recovery ratio of hard-elastic films.