It is well established that dramatic increases in conductivity occur upon the addition of conductive filler materials to highly resistive polymeric matrices in experimental settings. However, the mechanisms responsible for the observed behavior at low filler loadings, below theoretical percolation limits, of even high aspect ratio fillers such as carbon nanotubes (CNT) are not completely understood. In this study, conductive composites were fabricated using CNT bundles dispersed in epoxy resins at diverse loadings, using different dispersion and curing protocols. Based on electron microscopy observation of the CNTs strands distribution in the polymeric matrices and the corresponding electrical conductivities of those specimens, we concluded that no single electron transfer model can accurately explain the conductive behavior for all the loading values. We propose the existence of two different conductive mechanisms; one that exists close to the percolation limit, from ‘low loadings’ to higher CNT contents (CNT % wt > 0.1) and a second for ‘extremely low loadings’, near the percolation threshold (CNT % wt < 0.1). The high conductivity observed for composites at low CNT loading values can be explained by the existence of a percolative CNT network that coexists with micron size regions of non-conductive material. In contrast, samples with extremely low CNT loading values, which present no connectivity or close proximity between CNT bundles, show an electrical conductivity characterized by a current/voltage dependence. Data suggests that at these loadings, conduction may occur via a material breakdown mechanism, similar to dielectric breakdown in a capacitor. The lessons learned from the data gathered in here could guide future experimental research aimed to control the conductivity of CNT composites.
In this study, carbon nanotube (CNT) epoxy composite films were fabricated, characterized, and tested as resonant, plasmonic metamaterials. CNT–epoxy formulations, containing diverse CNT loadings, were fabricated and templates were used to generate repeating arrays of squares of diverse dimensions. Their absorption characteristics were characterized by collecting free space reflectivity data in the microwave band, using an arch setup in an anechoic chamber. Data were collected from 2 to 20 GHz. The materials behavior was modeled using a standard unit-cell-based finite element model, and the experimental and calculated data were compared. The experimental results were successfully reproduced with appropriate adjustments to relative permittivity of the composite films. This research demonstrates the ability to use CNT-based conductive composites for manufacturing metamaterials, offering a potentially lighter-weight alternative in place of traditional metal films. Lower conductivity than other conductors causes a widening of the absorption curves, providing a wider band of frequency absorption.
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