Filler network structure in graphene nanoplatelet (GNP)-filled polymethyl methacrylate (PMMA) composites: From thermorheology to electrically and thermally conductive properties

Abstract In this work, graphene nanoplatelet (GNP) filled polymethyl methacrylate (PMMA) composites were prepared using solution method via a specially designed route and relatively high thermal conductivities of the composites were achieved at a low GNP loading. The effect of GNP content on rheological behavior, thermal and electrical conductivity of the composites was intensively investigated. Thermorheological complexity was displayed at elevated GNP loading, and the rheological percolation threshold of GNP in PMMA decreased from 7.96 wt% at 220 °C to 4.02 wt% at 260 °C according to Winter-Chambon method, suggesting that GNP was more likely to form a seepage network at higher temperature. The DMTA results showed that the increase in moduli of the composites should be ascribed to the formation of the GNP-GNP network structure. The electrical conductivity of the composites underwent a sudden jump by seven orders of magnitude, which also indicated the formation of a GNP conductive pathway in the matrix with an electrical percolation threshold of 2–4 wt%. The results of transient temperature measurement were in good consistent with the thermal conductivity versus GNP loading, which was compared with various thermal conduction models with a modified Agari model presenting an acceptable evaluation of the dispersion status of GNP in the matrix. The experimental electrical and thermal conductivities as a function of GNP content could well be interpreted by the filler network structure as observed in morphological studies.