The Poly (arylene ether urea) Double Interface Layer Formed in PEEU@HfO2/PEI Nanocomposites Enables Enhanced Dielectric and Energy Storage Performance

Polyetherimide (PEI) has great potential as a dielectric because of its high-temperature resistance, but its low energy storage density limits practical applications. Incorporating hafnium dioxide (HfO2) with a moderate dielectric constant (k) and wide bandgap can simultaneously enhance the polarization intensity of PEI and potential barriers for charge injection. Nevertheless, the poor compatibility between HfO2 and PEI inevitably introduces defects, thereby weakening the inhibitory effect on dielectric loss. To tackle this issue, an organic double interface layer is introduced to enhance dielectric performance, where the polar poly(arylene ether urea) (PEEU) containing hydrogen bonds can ensure the layer's compactness. Notably, its non-bonding urea groups serve as deep traps to capture migrating carriers, and the gradient k values of HfO2, PEEU, and PEI help mitigate electric field distortions at the interface, therefore enhancing the suppression of conduction loss. The polarity of PEEU and the introduction of multiple interfaces significantly contribute to an increased k (maximum 9.7, at 1 kHz). At 300 kV mm−1, 5 vol% PEEU@HfO2/PEI achieves a discharged energy density of 3.3 J cm−3 and a high charge-discharge efficiency of 83%, surpassing 5 vol% HfO2/PEI by 1.95 and 2.44 times, respectively. The further COMSOL simulation verifies and proves this work as a novel design strategy for nanocomposite dielectrics.