Robust networks of interfacial localized graphene in cocontinuous polymer blends

Conductive polymer composites enjoy specialized applications such as electrostatic discharge protection. In this work, we create interfacially localized graphene nanoplatelets (GNPs) in a cocontinuous polymer blend of polylactide (PLA) and poly(ethylene-co-vinyl acetate) (EVA). Based on the wetting coefficient analysis, GNPs favor localization in the EVA phase. A two-step compounding sequence is designed such that a PLA/GNP masterbatch is first prepared via solution blending, and then melt compounded with the EVA. In the second step, GNPs transfer from the PLA phase to the EVA phase but become kinetically trapped at the interface, as confirmed by electron microscopy. We achieve an ultralow percolation threshold of 0.048 wt. % GNPs and obtain blends with electrical conductivities of ∼10⁻⁵ S/cm at 0.5 wt. % GNP concentration. We systematically study the shear and extensional rheology of the ternary composite system. Cocontinuous blends with interfacial GNPs exhibit higher shear and extensional viscosities compared to samples with GNPs localized entirely within the EVA phase. Rheology, in situ dielectric measurements, and transmission electron microscopic imaging after nonlinear deformations all show the interfacial GNP network undergoes structure recovery and largely remains at the PLA/EVA interface. Moreover, high electrical conductivity is maintained during 2-10 min melt compounding and conductivity recovers with annealing after nonlinear deformations. These results suggest that these robust GNP networks preserve their bulk electrical conductivity during subsequent melt processing.