Electrical modulus analysis on the Ni/CCTO/PVDF system near the percolation threshold

A type of Ni/CCTO/PVDF three-phase percolative composite was prepared, in which the filler content (volume fraction) of Ni and CCTO was set at 60 vol%. The dependence of permittivity, electrical modulus and ac conductivity on the concentration of Ni and CCTO fillers near the percolation threshold was investigated in detail. The permittivity of the composites dramatically increased as the Ni content approached 24 vol%. This unique physical mechanism was realized as the formation of conductive channels near the percolation threshold. Analysis on the electrical modulus showed that the conductive channels are governed by three relaxation processes induced by the fillers (Ni, CCTO) and PVDF matrix, which are the interfacial polarization derived from the interfaces between fillers (Ni, CCTO) and PVDF matrix, and the polarization of CCTO ceramic filler and PVDF matrix. The conductivity behaviour with various Ni loadings and temperature suggested that the transition from an insulating to a conducting state should be induced by charge tunnelling between Ni–Ni particles, Ni–CCTO fillers and Ni–PVDF matrix. These findings demonstrated that the tunnelling conduction in the composite can be attributed to the unique physical mechanism near the percolation threshold.