Mullins effect in polyethylene and its dependency on crystal content: A network alteration model.

This contribution is focused on the Mullins effect in polyethylene. An ultra-low-density polyethylene with 0.15 crystal content, a low-density polyethylene with 0.3 crystal content and a high-density polyethylene with 0.72 crystal content are subjected to cyclic stretching over a large strain range. Experimental observations are first reported to examine how the crystal content influences the Mullins effect in polyethylene. It is found that the cyclic stretching is characterized by a stress-softening, a hysteresis and a residual strain, whose amounts depends on the crystal content and the applied strain. A unified viscohyperelastic-viscoelastic-viscoplastic constitutive model is proposed to capture the polyethylene response over a large strain range and its crystal-dependency. The macro-scale polyethylene response is decomposed into two physically distinct sources, a viscoelastic-viscoplastic intermolecular part and a viscohyperelastic network part. The local inelastic deformations of the rubbery amorphous and crystalline phases are considered by means of a micromechanical treatment using the volume fraction concept. Experimentally-based material kinetics are designed by considering the Mullins effect crystal-dependency and are introduced into the constitutive equations to capture the experimental observations. It is shown that the model is able to accurately reproduce the Mullins effect in polyethylene over a large strain range. The inherent deformation mechanisms are finally presented guided by the proposed constitutive model.

A two-phase hyperelastic-viscoplastic constitutive model for semi-crystalline polymers: application to polyethylene materials with a variable range of crystal fractions.

Polyethylene-based polymers as biomedical materials can contribute to a wide range of biomechanical applications. Therefore, it is important to identify, analyse, and predict with precision their mechanical behaviour. Polyethylene materials are semi-crystalline systems consisting of both amorphous and crystalline phases interacting in a rather complex manner. When the amorphous phase is in the rubbery state, the mechanical behaviour is strongly dependent on the crystal fraction, therefore leading to essentially thermoplastic or elastomeric responses. In this study, the finite deformation stress-strain response of polyethylene materials is modelled by considering these semi-crystalline polymers as two-phase heterogeneous media in order to provide insight into the role of crystalline and amorphous phases on the macro-behaviour and on the material deformation resistances, i.e. intermolecular and network resistances. A hyperelastic-viscoplastic model is developed in contemplation of representing the overall mechanical response of polyethylene materials under large deformation. An evolutionary optimization procedure based on a genetic algorithm is developed to identify the model parameters at different strain rates. The identification results show good agreement with experimental data, demonstrating the usefulness of the proposed approach: the constitutive model, with only one set of identified parameters, allows reproducing the stress-strain behaviour of polyethylene materials exhibiting a wide range of crystallinities, the crystal content becoming the only variable of the model.