Hybrid carbon nanotube composites with two different types of fillers have attracted considerable attention for various advantages. The incorporation of micro-scale secondary fillers creates an excluded volume that leads to the increase in the electrical conductivity. By contrast, nano-scale secondary fillers shows a conflicting behavior of the decreased electrical conductivity with micro-scale secondary fillers. Although several attempts have been made in theoretical modeling of secondary-filler composites, the knowledge about how the electrical conductivity depends on the dimension of secondary fillers was not fully understood. This work aims at comprehensive understanding of the size effect of secondary particulate fillers on the electrical conductivity, via the combination of Voronoi geometry induced from Swiss cheese models and the underlying percolation theory. This indicates a transition in the impact of the excluded volume, i.e., the adjustment of the electrical conductivity was measured in cooperation with loading of second fillers with different sizes.

In response to the rising need for flexible and lightweight materials capable of efficient heat transport, many studies have been conducted to improve the thermal properties of polymers via nanofillers. Among the various nanofillers, carbon nanotubes (CNTs) are considered as the most promising, owing to their excellent thermal and electrical properties. Accordingly, CNT/polymer composites can be used as flexible and lightweight heat transfer materials, owing to their low density. In this study, we fabricated multi-walled CNT (MWCNT)/polymer composites with different aspect ratios to investigate their effects on electrical and thermal properties. Through a three-roll milling process, CNTs were uniformly dispersed in the polymer matrix to form a conductive network. Enhanced electrical and thermal properties were observed in MWCNT composite with a high aspect ratio as compared to those with a low aspect ratio. The thermal conductivity of composites obtained as a function of the filler content was also compared with the results of a theoretical prediction model.

Zero temperature coefficient of resistance (TCR) is essential for the precise control of temperature in heating element and sensor applications. Many studies have focused on developing zero-TCR systems with inorganic compounds; however, very few have dealt with developing zero-TCR systems with polymeric materials. Composite systems with a polymer matrix and a conducting filler show either a negative (NTC) or a positive temperature coefficient (PTC) of resistance, depending on several factors, e.g., the polymer nature and the filler shape. In this study, we developed a hybrid conducting zero-TCR composite having self-heating properties for thermal stability and reliable temperature control. The bi-layer composites consisted of a carbon nanotube (CNT)-based layer having an NTC of resistance and a carbon black (CB)-based layer having a PTC of resistance which was in direct contact with electrodes to stabilize the electrical resistance change during electric Joule heating. The composite showed nearly constant resistance values with less than 2% deviation of the normalized resistance until 200 °C. The CB layer worked both as a buffer and as a distributor layer against the current flow from an applied voltage. This behavior, which was confirmed both experimentally and theoretically, has been rarely reported for polymer-based composite systems.

We report on a new principle yielding enhanced electromagnetic shielding, using as an example a composite comprised of carbon nanotubes (CNTs) integrated with a reactive ethylene terpolymer (RET). Such composites were synthesized through the chemical reaction of the functional groups on the CNT with the epoxy linkage of the RET polymer. The main advantages of these composites include good dispersion with low electrical percolation volume fractions (~0.1 volume%), yielding outstanding microwave shielding efficiency for electromagnetic interference applications. The shielding effectiveness was characterized for both single-walled and multiwalled CNT-based composites and was much enhanced in the former. The specific roles of absorption and reflection in determining the total shielding, as a function of the nanotube filling fraction, is also discussed.