Dielectric Relaxation in the Hybrid Epoxy/MWCNT/MnFe₂O₄ Composites

The electrical properties of epoxy/MWCNT (multi-walled carbon nanotubes)/MnFe₂O₄ hybrid composites loaded with MWCNTs (below, 0.09 vol.%, and above, 0.58 vol.%, percolation threshold) and varying concentrations of MnFe₂O₄ up to 10 vol.% were studied in a wide frequency range (20 Hz-40 GHz) at different temperatures (20 K-500 K). At low frequencies, the dielectric permittivity and the electrical conductivity of composites with fixed amounts of MWCNT are strongly dependent on MnFe₂O₄ content. For MWCNT concentrations above the percolation threshold (i.e., 0.58 vol.%), the electrical conductivity highly decreases with the increase of the MnFe₂O₄ fraction. In contrast, for the epoxy/MWCNT just below the onset of electrical conductivity (0.09 vol.% of MWCNTs), there exists an optimal concentration of MnFe₂O₄ inclusions (i.e., 0.025 vol.%), leading to a dramatic increase of the electrical conductivity by three orders of magnitude. The electrical transport in composites is mainly governed by electron tunneling at lower temperatures (below 200 K), and it is highly impacted by the matrix conductivity at higher temperatures (above 400 K). The electrical properties were discussed in terms of the Maxwell-Wagner relaxation and distributions of relaxation times. A non-invasive platform based on dielectric relaxation spectroscopy was proposed for enhancing the synergetic effect coursed by using multiple nanoinclusions in polymer composites just below the percolation threshold.