High-performance thermoplastic elastomers (TPEs), based on recycled high-density polyethylene (HD-PE R ), olefinic type ethylene-propylene-diene monomer rubber (EPDM), and ground tire rubber (GTR) treated with bitumen, were prepared by using dynamic vulcanization technology, and their structure-property relationships were investigated. It was established that special pretreatment of GTR by bitumen confers outstanding mechanical properties on the resulting TPEs. TPEs, containing GTR pretreated by bitumen, exhibit thermal behavior similar to that of the HDPE R /EPDM basic blend in the temperature region up to about 340°C. Rheological measurements showed that bitumen acts as an effective plasticizer for the GTR-containing TPEs. SEM, DSC, and DMTA results revealed improved adhesion between the particles of GTR treated by bitumen and the surrounding thermoplastic matrix, compared to that of the untreated GTR particles. It was concluded that bitumen acts as an effective devulcanizing agent in the GTR treatment stage. In the following steps of TPE production, bitumen acts simultaneously as a curing agent for the rubber components (EPDM/GTR) and as a compatibilizer for the blend components. GTR-containing TPEs, prepared by extrusion technology, were reprocessed (by passing through the extruder six times) without any observable changes in their tensile properties, thermal stability, and melt viscosity.

Recycled low density polyethylene (R-LDPE) has been reactively compatibilized with butadiene rubber (BR) by using small additions of reactive polyethylene copolymers and reactive BRs to produce thermoplastic elastomers (TPEs). TPEs were characterized by thermogravimetric analysis (TGA), differential scanning calorimetry (DSC), dynamic mechanical analysis (DMA), rheology measurements, wide-angle X-ray scattering (WAXS) and mechanical testing. WAXS results show that the presence of BR and reactive modifiers does not completely prevent the crystallization of R-LDPE during the TPE formation. Depression of the melting point has been found in all cases. Also in all cases, compatibility is provided by formation of interfacial layers. The best mechanical characteristics are obtained for R-LDPE + BR blends compatibilized with poly(ethylene-co-acrylic acid) (PE-co-AA) and polybutadiene terminated with isocyanate groups (PB-NCO) for PB-NCO = 7.5 wt% per PB and COOH/NCO ratio = 1/1. The stress at break and elongation at break are respectively improved by 31 % and 63 %. The PB-NCO modifier participates in co-vulcanization with BR in the rubber phase and reacts at the interface with the PE-co-AA dissolved in the polyolefin phase. As a result, the amorphous phase of R-LDPE is dissolved by the rubber phase and a morphology with dual phase continuity is formed, assuring an improvement of mechanical properties of TPEs.