Abstract
A numerical model is presented that describes all aspects of flow-induced crystallization of isotactic polypropylene at high shear rates and elevated pressures. It incorporates nonlinear viscoelasticity, including viscosity change as a result of formation of oriented fibrillar crystals (shish), compressibility, and nonisothermal process conditions caused by shear heating and heat release as a result of crystallization. In the first part of this chapter, the model is validated with experimental data obtained in a channel flow geometry. Quantitative agreement between experimental results and the numerical model is observed in terms of pressure drop, apparent crystallinity, parent/daughter ratio, Hermans’ orientation, and shear layer thickness. In the second part, the focus is on flow-induced crystallization of isotactic polypropylene at elevated pressures, resulting in multiple crystal phases and morphologies. All parameters but one are fixed a priori from the first part of the chapter. One additional parameter, determining the portion of β-crystal spherulites nucleated by flow, is introduced. By doing so, an accurate description of the fraction of β-phase crystals is obtained. The model accurately captures experimental data for fractions of all crystal phases over a wide range of flow conditions (shear rates from 0 to 200 s−1, pressures from 100 to 1,200 bar, shear temperatures from 130°C to 180°C). Moreover, it is shown that, for high shear rates and pressures, the measured γ-phase fractions can only be matched if γ-crystals can nucleate directly on shish.
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Notes
- 1.
- 2.
For these phases orientation might decrease crystal growth rate; however, there is no experimental evidence for this effect.
- 3.
For shear undercooling of 30°C, the shear pulse is visible as a temporary dip in the specific volume. For shear undercooling of 60°C, crystallization occurs during the shear pulse and therefore the dip is not visible.
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Appendix: Model Without Increase in α-Growth Rate as a Result of Orientation
Appendix: Model Without Increase in α-Growth Rate as a Result of Orientation
Figure 21 shows calculations for the volume fractions of α- and γ-phases for the case that the γ-phase can nucleate directly on shish to form kebabs, with no increase in α-growth rate during and shortly after flow as a result of orientation (i.e., G flow = 0 in Eq. 36). It is observed that the eight data points highlighted in Sect. 4.2.3 now all collapse on the, approximately, linear relation between crystal volume fraction and crystallization temperature. This is an indication that the deviation from this trend is caused by the α-phase having an increased growth rate as a result of orientation caused by flow.
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Roozemond, P.C., van Drongelen, M., Peters, G.W.M. (2016). Modeling Flow-Induced Crystallization. In: Auriemma, F., Alfonso, G., de Rosa, C. (eds) Polymer Crystallization II. Advances in Polymer Science, vol 277. Springer, Cham. https://doi.org/10.1007/12_2016_351
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