Anomalous Conductive Properties of Polymer Composites with Carbon Nanotubes: Why Power Laws Are Not Universal

Abstract

The conductive properties of CNT/polymer composites have been extensively studied. However, the impact of CNT distribution in the matrix on the composite polarization remains underexplored and poorly understood. Since it is difficult to achieve a uniform distribution of CNTs in polymers, most researchers have focused only on indiscriminately aggregated states. In this article, a new blending method was suggested to prepare a series of epoxy resin-based composite samples with varying levels of CNT uniformity/aggregation and the same filling fractions. Notably, the permittivity values turned out to be inversely related to the composite uniformity: the lowest permittivity values were obtained in the most uniform formulation, and vice versa. With 0.1% CNT, the real part values of the most uniform and aggregated samples were 6.6 and 16.2 at 107 Hz and 11.6 and 370.5 at 101 Hz, respectively. For the filler content of 0.1–0.5%, the conductive properties were largely determined by the distribution of CNTs and not their content. Within the entire frequency range, the uniform sample with 0.2% CNT exhibited significantly lower permittivity than the aggregated sample with 0.1% CNT. These findings emphasize the importance of the aggregation factor and underscore the non-universality and limitations of the percolation theory and power laws. The observed phenomenon is best explained by the micro-capacitor model, or the Maxwell–Wagner polarization, and suggests that a significant portion of the literature in the field needs to be reconsidered.