Dielectric relaxation dynamics of high-temperature piezoelectric polyimide copolymers

Polyimide copolymers have been prepared based on different diamines as comonomers: a diamine without CN groups and a novel synthesized diamine with two CN groups prepared by polycondensation reaction followed by thermal cyclodehydration. Dielectric spectroscopy measurements were performed, and the dielectric complex function, ac conductivity and electric modulus of the copolymers were investigated as a function of CN group content in the frequency range from 0.1 to 10 7 Hz at temperatures from 25 to 260 °C. For all samples and temperatures above 150 °C, the dielectric constant increases with increasing temperature due to increasing conductivity. The α-relaxation is just detected for the sample without CN groups, being this relaxation overlapped by the electrical conductivity contributions in the remaining samples. For the copolymer samples and the polymer with CN groups, an important Maxwell–Wagner–Sillars contribution is detected. The mechanisms responsible for the dielectric relaxation, conduction process and electric modulus response have been discussed as a function of the CN group content present in the samples.