The effect of temperature and graphene concentration on the electrical conductivity and dielectric permittivity of graphene–polymer nanocomposites

Several recent experiments have revealed the remarkable influence of temperature and graphene concentration on the effective electrical properties of graphene–polymer nanocomposites, but no theory seems to exist at present to quantify such dependence. In this work, we develop a novel micromechanics-based homogenization scheme to connect the microstructural features of constituent phases to the temperature-dependent macroscopic conductivity and permittivity for the nanocomposites. The key microstructural features include the graphene volume concentration, temperature-dependent electrical properties of constituent phases, percolation threshold, imperfect mechanical bonding effect with temperature-degraded interlayer, and the temperature-dependent electron tunneling and Maxwell–Wagner–Sillars polarization. We consider the activation of free electrons and polarization of molecules to write the constitutive equations of polymer, and the collision and vibration probabilities to write those of graphene. We highlight the developed theory with a direct comparison to the experimental data of rGO/epoxy nanocomposites over the temperature range from 293 to 353 K. It shows that before the percolation threshold, the effective electrical conductivity and dielectric permittivity markedly increase with temperature, but after the percolation threshold, the influence of temperature diminishes significantly. In the latter case, the effective permittivity increases only slightly, while the conductivity exhibits an opposite trend.