Localizing graphene at the interface of cocontinuous polymer blends: Morphology, rheology, and conductivity of cocontinuous conductive polymer composites

Interfacial localization of graphene in cocontinuous polymer blends is shown to be effective in stabilizing the cocontinuous morphology and increasing conductivity with a low electrical percolation threshold. We created polylactic acid (PLA) and polystyrene (PS) cocontinuous blends filled with thermally reduced graphene oxide (r-GO) localized at the interface. The resulting conductive composites show dramatically improved conductivity at low filler loadings and an ultralow percolation threshold of 0.028 vol. %. We systematically studied the changes of conductivity and rheology of the PLA-PS composites during annealing. We found that r-GO transfers from the PLA phase to the interface during melt compounding and annealing and forms a spanning 3D network, which effectively suppresses the coarsening of the cocontinuous structure. Our study demonstrated that the 3D r-GO network significantly increases the conductivity and the storage modulus of the melt blends. Finally, we constructed a simple model, which quantitatively explains the correlations between structural, electrical, and rheological properties of conductive polymer composites.