Fabrication and origin of high-k carbon nanotube/epoxy composites with low dielectric loss through layer-by-layer casting technique

The distribution of polarized space charges and their relaxation behavior in high dielectric constant electric conductor/polymer composites are main factors that determine the frequency-dependent dielectric constant and dielectric loss. However, few reports focus on this motif. We present here the dielectric performance and mechanism of a unique kind of composites with multi-layers (coded as [MWCNT/EP]x, where x refers to the number of layers), fabricated by using layer-by-layer casting technique. Each composite layer with same thickness was composed of multi-walled carbon nanotubes (MWCNTs) and epoxy (EP) resin. When the loading of MWCNTs is 0.5 wt%, the four-layer [MWCNT0.5/EP]4 material shows the highest dielectric constant (465 at 1 Hz) and low dielectric loss tangent (0.7 at 1 Hz), about 4 and 2.1 × 10−2 times the values of traditional MWCNT0.5/EP composite, respectively. By investigating the space charge polarization (SCP), Debye polarization and dielectric moduli in [MWCNT/EP]x materials, the complex relationships and the origin among dielectric constant, dielectric loss, frequency and the content of filler were clearly elucidated. The SCP within each layer is different from that between layers. The greatly improved dielectric properties of [MWCNT/EP]x materials are believed to be the reinforced SCP and blocked transport of carriers between every two layers.