Rational Design of Two-Step Functionalized Barium Titanate for Improving Dielectric Properties of poly(Arylene Ether Nitrile) Composites

Ceramic/polymer dielectrics with excellent thermal stability and high dielectric performance exhibit great potential in advanced capacitor applications. It is still a major challenge for ceramic/polymer dielectrics to obtain high dielectric constant at low content while maintaining excellent flexibility. To alleviate this issue, here, a flexible polymer dielectric composite consisting of poly(arylene ether nitrile) (PEN) matrix and barium titanate filler coated by Carbon and polypyrone (h-BT@C@PPy) was put forward in this work. The as-prepared composite films displayed high dielectric constant, comparable low loss and favorable interfacial binding due to the hydrogen-bonding interaction between –NH of h-BT@C@PPy and –CN of PEN, effectively promoting the interfacial polarization and remedying the internal interface defects between h-BT and PEN. Consequently, an addition of 8 wt% h-BT@C@PPy into PEN matrix raised the dielectric constant from 3.82 to 13.3 at 1 kHz, while maintaining relatively low dielectric loss (0.05@1 kHz). However, the breakdown strength showed a decreasing trend with the lowest value of 60.37 kV mm⁻¹. Meanwhile, the better flexibility, outstanding thermal stability (the 5% weight loss above 500 °C) as well as excellent permittivity-temperature stability was also delivered by the PEN-based composite films. This strategy furnishes a perspective to design ceramic/polymer dielectrics with high-k achieved at low filler content for the applications of organic film capacitors.