Hydrogen Bonding of Aramid Boosts High-Temperature Capacitive Properties of Polyetherimide Blends

Polyetherimide (PEI) is the state-of-the-art commercial high-temperature polymer dielectric with excellent thermal and chemical stability and relatively high high-temperature capacitive energy storage properties. The rotation of the dipoles in the PEI chains brings the β-relaxation which seriously increases the leakage current and decreases the charge-discharge efficiency. In this work, hydrogen bonds have been introduced to limit the dipole rotation of PEI by blending aramids [1,4-poly(ether fluoromethyl naphthalene amide), PNFA] into the PEI matrix. By introducing 10 wt % PNFA, the β-relaxation of the blend has been significantly reduced which could be observed from the dielectric spectrum. To explore the mechanism of limited β-relaxation, we analyze the hydrogen bonds in the blend films by infrared spectroscopy and found that the maximum content of hydrogen-bonded carbonyl formed between PNFA and PEI chains was 14.3% when the content of PNFA was 30 wt %. The content of hydrogen bonds formed between PNFA and PEI was positively correlated with the energy storage performance of the blends. The maximum discharged energy density with an efficiency above 90% of the blend film with 30 wt % PNFA reaches 4.1 J cm^-3 at 150 °C, which is about 350% higher than that of pristine PEI. This work shows that composing hydrogen bonds by the blending method could be a viable strategy for enhancing the high-temperature energy storage performance of polymer dielectrics, which could be achieved by large-scale preparation and has feasible industrial production prospects.