Dynamically crosslinked thermoplastic elastomer nanocomposites were synthesized as modifier for the bitumen binder-based asphalts. Linear low-density polyethylene (LLDPE) and styrene-butadiene rubber (SBR), with the ratio of 80/20, bitumen, and organically modified clay (OC) were all melt mixed in the presence of the sulfur curing system. The proposed mixing was carried out in an internal mixer at 160 °C with a rotor speed of 120 rpm. To enhance the molecular interactions between the polymer phases and the clay silicate layers, maleic anhydride-grafted LLDPE (PE-g-MA) with the maleiation degree of 50% was also incorporated into the mixture. Observation of the composite samples, using the scanning electron microscopy (SEM), revealed the matrix dispersed type of morphology for all dynamically vulcanized samples. X-ray diffraction (XRD) and transmission electron microscopy (TEM) examinations evidenced the exfoliation of the clay silicate layers with good dispersion. Rheomechanical spectrometry (RMS) was performed on the prepared nanocomposites. All dynamically vulcanized nanocomposites comprising 2.5% of OC exhibited shear-thinning behavior and non-terminal characteristics with a low frequency range. These indicate the formation of three-dimensional physical networks by the clay nanolayers throughout the LLDPE matrix. The presence of the bitumen in the composition of the prepared nanocomposites improved the flowability of the samples. This is a promising feature of the prepared nanocomposites to be used as an elastic and resistant modifier in the composition of the bitumen-based asphalts.
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