Polyphenylene Oxide Film Sandwiched between SiO2 Layers for High-Temperature Dielectric Energy Storage.

The commercial capacitor using dielectric biaxially oriented polypropylene (BOPP) can work effectively only at low temperatures (less than 105 °C). Polyphenylene oxide (PPO), with better heat resistance and a higher dielectric constant, is promising for capacitors operating at elevated temperatures, but its charge-discharge efficiency (η) degrades greatly under high fields at 125 °C. Here, SiO2 layers are magnetron sputtered on both sides of the PPO film, forming a composite material of SiO2/PPO/SiO2. Due to the wide bandgap and high Young's modulus of SiO2, the breakdown strength (Eb) of this composite material reaches 552 MV/m at 125 °C (PPO: 534 MV/m), and the discharged energy density (Ue) under Eb improves to 3.5 J/cm3 (PPO: 2.5 J/cm3), with a significantly enhanced η of 89% (PPO: 70%). Furthermore, SiO2/PPO/SiO2 can discharge a Ue of 0.45 J/cm3 with an η of 97% at 125 °C under 200 MV/m (working condition in hybrid electric vehicles) for 20,000 cycles, and this value is higher than the energy density (∼0.39 J/cm3 under 200 MV/m) of BOPP at room temperature. Interestingly, the metalized SiO2/PPO/SiO2 film exhibits valuable self-healing behavior. These results make PPO-based dielectrics promising for high-temperature capacitor applications.

γ-Ray Irradiation Significantly Enhances Capacitive Energy Storage Performance of Polymer Dielectric Films.

Polymer dielectric capacitors are fundamental in advanced electronics and power grids but suffer from low energy density, hindering miniaturization of compact electrical systems. It is shown that high-energy and strong penetrating γ-irradiation significantly enhances capacitive energy storage performance of polymer dielectrics. γ-irradiated biaxially oriented polypropylene (BOPP) films exhibit an extraordinarily high energy density of 10.4 J cm-3 at 968 MV m-1 with an efficiency of 97.3%. In particular, an energy density of 4.06 J cm-3 with an ultrahigh efficiency of 98% is reliably maintained through 20 000 charge-discharge cycles under 600 MV m-1. At 125 °C, the γ-irradiated BOPP film still delivers a high discharged energy density of 5.88 J cm-3 with an efficiency of 90% at 770 MV m-1. Substantial improvements are also achieved for γ-irradiated cycloolefin copolymers at a high temperature of 150 °C, verifying the strategy generalizability. Experimental and theoretical analyses reveal that the excellent performance should be related to the γ-irradiation induced polar functional groups with high electron affinity in the molecular chain, which offer deep energy traps to impede charge transport. This work provides a simple and generally applicable strategy for developing high-performance polymer dielectrics.

Coexistence of Both Localized Electronic States and Electron Gas at Rutile TiO2 Surfaces.

Localized electron polarons formed through the coupling of excess electrons and ionic vibrations play a key role in the functionalities of materials. However, the mechanism of the coexistence of delocalized electrons and localized polarons remains underexplored. Here, the discovery of high-mobility 2D electron gas at the rutile TiO2 surfaces through argon ion irradiation induced oxygen vacancies is reported. Strikingly, the electron gas forms localized electronic states at lower temperatures, resulting in an abrupt metal-insulator transition. Moreover, it is found that the low-temperature conductivity in the insulating state is dominated by excess free electrons with a high mobility of ≈103 cm2 V-1 s-1 , whereas the carrier density is dramatically suppressed with decreasing temperature. Remarkably, it reveals that the application of an electric field can lead to a collapse of the localized states, resulting in a metallic state. These results reveal the strongly correlated/coupled nature between the localized electrons and high-mobility electrons and offer a new pathway to probe and harvest the exotic electron states at the complex oxide surfaces.

Influence of In-Gap States on the Formation of Two-Dimensional Election Gas at ABO3/SrTiO3 Interfaces.

We explored in-gap states (IGSs) in perovskite oxide heterojunction films. We report that IGSs in these films play a crucial role in determining the formation and properties of interfacial two-dimensional electron gas (2DEG). We report that electron trapping by IGSs opposes charge transfer from the film to the interface. The IGS in films yielded insulating interfaces with polar discontinuity and explained low interface carrier density of conducting interfaces. An ion trapping model was proposed to explain the physics of the IGSs and some experimental findings, such as the unexpected formation of 2DEG at the initially insulating LaCrO3/SrTiO3 interface and the influence of substitution layers on 2DEG.