The objective of this work is to study the influence of the ratio between the elastomer (EPDM) phase and the thermoplastic phase (PP) in thermoplastic vulcanizates (TPVs) as well as the associated morphology of the compression set of the material. First, from a study of the literature, it is concluded that the rubber phase must be dispersed with a large distribution of the domain size in the thermoplastic phase in order to achieve a high concentration, i.e., a maximal packing fraction close to ~0.80. From this discussion, it is inferred that a certain degree of progress in the crosslinking reaction must be reached when the thermoplastic phase is melted during mixing in order to achieve dispersion of the elastomeric phase in the thermoplastic matrix under maximum stress. In terms of elasticity recovery which is measured from the compression set experiment, it is observed that the crosslinking agent nature (DCP or phenolic resin) has no influence in the case of a TPV compared with a pure crosslinked EPDM system. Then, the TPV morphology and the rubber phase concentration are the first order parameters in the compression set of TPVs. Finally, the addition of carbon black fillers leads to an improvement of the mechanical properties at break for the low PP concentration (20%). However, the localization of carbon black depends on the crosslinking chemistry nature. With radical chemistry by organic peroxide decomposition, carbon black is located at the interface of EPDM and PP acting as a compatibilizer.
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