To better understand the processing and final properties
of multilayer
films obtained by layer forced assembly in coextrusion as well as
their structure morphology, the present study focuses on model films
with LDPE as the base polymer. More specifically, the layer confinement
of LDPE by a glassy amorphous polymer (here, PC or PS) was investigated.
First, the viscosity and elasticity ratios of the different neat polymers
were measured by rheological tests to simulate the processing conditions
in the feedblock and multipliers during coextrusion. These results
together with the observation of film transparency at the macroscopic
scale and the layer breakup phenomena between layers at the microscopic
scale enabled us to build a comprehensive stability map rationalizing
the conditions required for a well-controlled multinanolayer architecture.
Second, the morphology of the coextruded films was analyzed by SEM
and TEM. The onset of the layer breakup in the LDPE/PS system was
determined at 2048 layers with a layer thickness of 95 nm, while in
the LDPE/PC system, it was at 256 layers with a layer thickness of
980 nm. The layer breakup happened at a fewer number of layers for
the LDPE/PC system due to the viscoelastic mismatched properties between
the base polymers. Interestingly, we have demonstrated that it is
nonetheless possible to prepare some nanolayer structures with 16,380
layers of the PS/LDPE system with some defects but still maintain
an overall property improvement despite their high mismatched viscoelastic
properties. Finally, the orientation and crystalline structure of
the coextruded films were characterized by 2D-WAXS and DSC, and the
ultimate properties of the films were determined through tensile testing.
The geometrical confinement of the LDPE nanolayer did not affect the
thermal crystalline properties of LDPE chains, but it affected the
crystalline morphologies as well as the final mechanical response
of the obtained multilayer films.