RESUMEN
High-temperature polymer dielectrics have broad application prospects in next-generation microelectronics and electrical power systems. However, the capacitive energy densities of dielectric polymers at elevated temperatures are severely limited by carrier excitation and transport. Herein, a molecular engineering strategy is presented to regulate the bulk-limited conduction in the polymer by bonding amino polyhedral oligomeric silsesquioxane (NH2 -POSS) with the chain ends of polyimide (PI). Experimental studies and density functional theory (DFT) calculations demonstrate that the terminal group NH2 -POSS with a wide-bandgap of Eg ≈ 6.6 eV increases the band energy levels of the PI and induces the formation of local deep traps in the hybrid films, which significantly restrains carrier transport. At 200 °C, the hybrid film exhibits concurrently an ultrahigh discharged energy density of 3.45 J cm-3 and a high gravimetric energy density of 2.74 J g-1 , with the charge-discharge efficiency >90%, far exceeding those achieved in the dielectric polymers and nearly all other polymer nanocomposites. Moreover, the NH2 -POSS terminated PI film exhibits excellent charge-discharge cyclability (>50000) and power density (0.39 MW cm-3 ) at 200 °C, making it a promising candidate for high-temperature high-energy-density capacitors. This work represents a novel strategy to scalable polymer dielectrics with superior capacitive performance operating in harsh environments.
RESUMEN
Polymer film capacitors have been widely used in electronics and electrical power systems due to their advantages of high power densities, fast charge-discharge speed, and great stability. However, the exponential increase of electrical conduction with temperature and applied electric field substantially degrades the capacitive performance of dielectric polymers at elevated temperatures. Here, the first example of controlling the energy level of charge traps in all-organic crosslinked polymers by tailoring molecular structures that significantly inhibit high-field high-temperature conduction loss, which largely differs from current approaches based on the introduction of inorganic fillers, is reported. The polymer network with optimized crosslinking structures exhibits an ultrahigh discharged energy density of 7.02 J cm-3 with charge/discharge efficiencies of >90% at 150 °C, far outperforming current dielectric polymers and composites. The charge-trapping effects in different crosslinked structures, as the origins of the marked improvements in the high-temperature capacitive performance, are comprehensively investigated experimentally and confirmed computationally. Moreover, excellent cyclability and self-healing features are demonstrated in the polymer film capacitors. This work offers a promising pathway of molecular structure design to scalable high-energy-density polymer dielectrics capable of operating under harsh environments.
RESUMEN
Polymer dielectrics have drawn tremendous attention worldwide due to their huge potential for pulsed power capacitors. Recent studies have demonstrated that linear/nonlinear layered composites, which can effectively balance energy density and efficiency, have huge potential for capacitive energy storage applications. However, further enhanced energy densities are strongly desired to meet the everincreasing demand for the miniaturization of electronic devices. Herein, a novel class of core-shell structured graphene@titanium dioxide nanoboxes is successfully synthesized and introduced into poly(vinylidene fluoride-hexafluoropropylene)-poly(ether imide) double-layer films. It is exciting to find that the introduction of merely 0.5 wt % nanoboxes results in a substantially enhanced energy density of 19.39 J/cm3, which is over 2.6 times that of the film without nanoboxes (7.44 J/cm3). Meanwhile, a high breakdown strength of 655 kV/mm and a high efficiency of 83% are achieved. Furthermore, the nanocomposites also show excellent power densities and cycling stabilities. These composites with excellent comprehensive energy storage performances have huge potential for advanced pulsed power capacitors.
RESUMEN
A new general method for the fabrication of a reduced graphene oxide (rGO)-based ordered monolayer macroporous film composed of a layer of closely arranged pores is introduced. Assisted by the polystyrene microsphere monolayer colloid crystal by a simple solution-heated method, pure rGO, rGO-SnO2, rGO-Fe2O3, and rGO-NiO composite monolayer ordered porous films were examplarily constructed on the curved surface of a ceramic tube widely used in gas sensors. The rGO-oxide composite porous films could exhibit much better sensing performances than those of the corresponding pure oxide films and the composite films without the ordered porous structures in detecting ethanol gas. The enhancement mechanisms induced by distinctive rGO-oxide heterojunctions and porous structures as well as the effects of the rGO content and the pore-size on the sensitivity of the composite films were systematically analyzed and discussed. This study opens up a kind of construction method for an rGO-based composite film gas sensor with uniform surface structures and high performance.
RESUMEN
A new graphene-based composite structure, monolayer-ordered macroporous film composed of a layer of orderly arranged macropores, was reported. As an example, SnO2-reduced graphite oxide monolayer-ordered macroporous film was fabricated on a ceramic tube substrate under the irradiation of ultra-violet light (UV), by taking the latex microsphere two-dimensional colloid crystal as a template. Graphite oxide sheets dispersed in SnSO4 aqueous solution exhibited excellent affinity with template microspheres and were in situ incorporated into the pore walls during UV-induced growth of SnO2. The growing and the as-formed SnO2, just like other photocatalytic semiconductor, could be excited to produce electrons and holes under UV irradiation. Electrons reduced GO and holes adsorbed corresponding negative ions, which changed the properties of the composite film. This film was directly used as gas-sensor and was able to display high sensitivity in detecting ethanol gas. More interestingly, on the basis of SnO2-induced photochemical behaviours, this sensor demonstrated tunable sensitivity when UV irradiation time was controlled during the fabrication process and post in water, respectively. This study provides efficient ways of conducting the in situ fabrication of a semiconductor-reduced graphite oxide film device with uniform surface structure and controllable properties.