Abstract

Bio-based graphene-reinforced thermoplastic elastomers (TPE) based on natural rubber (NR), and poly lactic acid (PLA) were successfully prepared via melt blending. The effect of graphene nanosheets (GNS) content and coupling agent were investigated on morphological, thermal and rheological properties of the PLA/NR/GNS bio-nanocomposites. More stable morphology of uniformly dispersed NR phase in the continuous PLA matrix with a relatively narrower diameter-size distribution was achieved in the presence of a compatibilizer. Moreover, transmission electron micrographs showed more improved dispersion of GNS with predominantly exfoliated morphology in the case of ENR-compatibilized PLA/NR/GNS bio-nanocomposites. Crystallization/melting studies revealed that, as the GNS content increased, the cold-crystallization peak, melting peak and glass-to-rubber transition temperature values shifted to higher temperatures and the crystallinities of blends slightly decreased (about 7%) which might be attributed to the reduction of polymeric segments mobility by the restricting effect of GNS. Dynamical mechanical investigation showed that the storage modulus (E′) increased about 25% by the introduction of GNS due to the inherent stiffness of GNS and the occurrence of compatibility in the PLA/NR blend in the presence of ENR. The presence of ENR shifted the $$ T_{g} $$ of the NR phase and the PLA matrix towards each other which is a characteristic of higher miscibility and compatibility. The thermogravimetry (TGA) and derivative thermogravimetry (DTG) curves revealed higher thermal stability of the compatibilized-PLA/NR blends due to the enhanced interfacial adhesion and the homogenous dispersion of GNSs as direct effects of the presence of ENR. Rheological studies indicated that the formation of the effective GNS-polymer networks by the presence of ENR increased the storage modulus (G′) and complex viscosity (η*) value due to the effectiveness of the GNS in taking loads and restricted molecular motion, respectively.

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