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Article Dans Une Revue Journal of Physical Chemistry B Année : 2022

Modeling Method for Semi-crystalline Polymers Controlling Aspects of the Morphology at the Molecular Scale for the Study of Mechanical and Physicochemical Properties

Résumé

A novel method is presented to build semi-crystalline polymer models used in molecular dynamics simulations. The method allows controlling certain aspects of the molecu- lar morphology of the material. It relies on the generation of the polymer sections in the amorphous phase of the semi-crystalline structure according to the statistical polymer physics theory proposed by Adhikari and Muthukumar [Adhikari S. and Muthukumar M., J. Chem. Phys., 2019 151, 114905]. The amorphous phase is first built based on the method initially developed by Theodorou and Suter [Theodorou D. N. and Suter U. W., Macromolecules 1985 18 (7), 1467-1478]. Then, the amorphous phase is stacked between crystallites, and a connection algorithm proposed by Rigby et al. [Rigby, D., Saxe, P.W., Freeman, C.M., Leblanc, B. Advanced Composites for Aerospace, Marine, and Land Applications. 2014 Springer, Cham], initially developed to build polymer thermosets, is employed to link the two phases. For a given set of degree of crystallinity, semi-crystalline long period, densities of the crystalline and amorphous phases and polymer molecular weight, the characteristic ratio is used to control the relative fractions of different types of polymer sections in the amorphous phase as well as the distribution of their lengths. There are three types of amorphous polymer sections: the ones that are reentering in the same crystallite called loops, those that are bonding two different crystallites called tie chains, and the chain tails ending in the amorphous region. The higher the imposed characteristic ratio is, the higher the fraction of tie chains is. The full implementation of the theory is described and then applied to High-Density PolyEthylene (HDPE). Several samples are generated. The obtained structures are characterized. Their elastic coeffcients are computed, and high uniaxial deformations are performed. It is shown that the higher the degree of crystallinity, the higher the elastic coeffcients. An entanglement analysis shows that the quantity of tie chains is more decisive than the entanglements in acting as stress transmitters to rigidify the structure.
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Dates et versions

hal-03854280 , version 1 (15-11-2022)

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Boris Belin, Marianna Yiannourakou, Véronique Lachet, Bernard Rousseau. Modeling Method for Semi-crystalline Polymers Controlling Aspects of the Morphology at the Molecular Scale for the Study of Mechanical and Physicochemical Properties. Journal of Physical Chemistry B, 2022, ⟨10.1021/acs.jpcb.2c04571⟩. ⟨hal-03854280⟩
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