Linear viscoelastic behavior of poly(ethylene terephtalate) above Tg amorphous viscoelastic properties Vs crystallinity: Experimental and micromechanical modeling

Linear viscoelastic behavior of amorphous and semicrystalline poly(ethylene terephtalate), (PET), was experimentally investigated. PET’s samples with different crystallinities (Xc) were prepared and viscoelastically characterized. Based on our experimental results (properties of the amorphous PET and semicrystalline polymers), micromechanical model was used to, first predict the viscoelastic properties of the semicrystalline polymers and second predict the changes on the viscoelastic properties of the amorphous phase when the crystallinity increases. For the micromechanical modeling of semicrystalline material’s viscoelastic properties, difficulties lie on the used numerical methods (Laplace-Carson transformation) and also on the actual physical and mechanical properties of the amorphous phase. In this paper we tried to simplify the Laplace-Carson-based method by using a pseudo-elastic one that avoids the numerical difficulties encountered before. The time-dependant problem is so replaced by a frequency-dependant set of elastic equations. Good agreement with low crystallinity fraction was found however large discrepancies appear for medium and high crystallinity. The poor agreement raises the issue of which amorphous mechanical properties should be taken as input in the micromechanical model? According to the dynamic mechanical analysis (DMA) experimental data, multiple amorphous phases with different glass transition temperatures were observed for each tested semicrystalline sample. For each sample, new glass transition temperature related to an equivalent amorphous phase was determined. DMA tests done at 1 Hz help estimating the mechanical properties of the new amorphous phase based on its new glass transition temperature. Using the new micromechanical approach developed in this paper, the changes occurring on the viscoelastic behavior of the amorphous phase upon crystallization were estimated. Good agreement was found after comparing the micromechanically estimated amorphous behavior with the experimentally estimated one leading to believe that the physical and mechanical properties of the amorphous phase change upon crystallization and taking on account this phenomenon is a key to a good prediction of the semicrystalline behavior using micromechanical models.