Asymmetric Trilayer All-Polymer Dielectric Composites with Simultaneous High Efficiency and High Energy Density: A Novel Design Targeting Advanced Energy Storage Capacitors

Polymeric dielectrics have attracted intensive attention worldwide because of their huge potential for advanced energy storage capacitors. Thus far, various effective strategies have been developed to improve the inherent low energy densities of polymer dielectrics. However, enhanced energy density is always accompanied by suppressed discharge efficiency, which is detrimental to practical applications and deserves considerable concern. Targeting at achieving simultaneous high energy density and high discharge efficiency, the unique design of asymmetric all-polymer trilayer composite consisting of a transition layer sandwiched by a linear dielectric layer and a nonlinear dielectric layer is herein reported. It is demonstrated that the nonlinear dielectric layer offers high energy density, while the linear dielectric layer provides high discharge efficiency. Especially, the transition layer can effectively homogenize the electric field distribution, resulting in greatly elevated breakdown strength and improved energy density. In particular, a high efficiency of 89.9% along with a high energy density of 12.15 J cm⁻³ are concurrently obtained. The asymmetric trilayer all-polymer design strategy represents a new way to achieve high-performance dielectric energy storage materials.     

Topological‐Structure Modulated Polymer Nanocomposites Exhibiting Highly Enhanced Dielectric Strength and Energy Density

Dielectric materials with high electric energy densities and low dielectric losses are of critical importance in a number of applications in modern electronic and electrical power systems. An organic–inorganic 0–3 nanocomposite, in which nanoparticles (0‐dimensional) are embedded in a 3‐dimensionally connected polymer matrix, has the potential to combine the high breakdown strength and low dielectric loss of the polymer with the high dielectric constant of the ceramic fillers, representing a promising approach to realize high energy densities. However, one significant drawback of the composites explored up to now is that the increased dielectric constant of the composites is at the expense of the breakdown strength, limiting the energy density and dielectric reliability. In this study, by expanding the traditional 0–3 nanocomposite approach to a multilayered structure which combines the complementary properties of the constituent layers, one can realize both greater dielectric displacement and a higher breakdown field than that of the polymer matrix. In a typical 3‐layer structure, for example, a central nanocomposite layer of higher breakdown strength is introduced to substantially improve the overall breakdown strength of the multilayer‐structured composite film, and the outer composite layers filled with large amount of high dielectric constant nanofillers can then be polarized up to higher electric fields, hence enhancing the electric displacement. As a result, the topological‐structure modulated nanocomposites, with an optimally tailored nanomorphology and composite structure, yield a discharged energy density of 10 J/cm³ with a dielectric breakdown strength of 450 kV mm^–1, much higher than those reported from all earlier studies of nanocomposites.     

Dual Support System Ensuring Porous Co–Al Hydroxide Nanosheets with Ultrahigh Rate Performance and High Energy Density for Supercapacitors

Layered double hydroxides (LDHs) are promising supercapacitor electrode materials due to their high specific capacitances. However, their electrochemical performances such as rate performance and energy density at a high current density, are rather poor. Accordingly, a facile strategy is demonstrated for the synthesis of the integrated porous Co–Al hydroxide nanosheets (named as GSP‐LDH) with dual support system using dodecyl sulfate anions and graphene sheets as structural and conductive supports, respectively. Owing to fast ion/electron transport, porous and integrated structure, the GSP‐LDH electrode exhibits remarkably improved electrochemical characteristics such as high specific capacitance (1043 F g^?1 at 1 A g^?1) and ultra‐high rate performance capability (912 F g^?1 at 20 A g^?1). Moreover, the assembled sandwiched graphene/porous carbon (SGC)//GSP‐LDH asymmetric supercapacitor delivers a high energy density up to 20.4 Wh kg^?1 at a very high power density of 9.3 kW kg^?1, higher than those of previously reported asymmetric supercapacitors. The strategy provides a facile and effective method to achieve high rate performance LDH based electrode materials for supercapacitors.     

Ultrahigh Breakdown Strength and Improved Energy Density of Polymer Nanocomposites with Gradient Distribution of Ceramic Nanoparticles

High‐energy‐density polymer nanocomposites with high‐dielectric‐constant ceramic nanoparticles as the reinforcement exhibit great potential for energy storage applications in modern electronic and electrical systems. However, the decline of breakdown strength by high loading of ceramic nanoparticles hinders this composite approach from sustainable promotion of energy density. In this work, an approach is proposed and demonstrated by constructing gradient distribution of the spherical ceramic nanoparticles in the polymer matrix. These gradient‐structured nanocomposites possess remarkably improved mechanical and electrical behaviors, which give rise to ultrahigh breakdown strength and much‐promoted energy density. Moreover, this enhancement effect can be further enlarged via increasing the grades number of gradient structures. This work provides an effective strategy for developing flexible high‐energy‐density polymer/ceramic nanocomposites for dielectric and energy storage applications.     

High‐Energy‐Density Dielectric Polymer Nanocomposites with Trilayered Architecture

The development of advanced dielectric materials with high electric energy densities is of crucial importance in modern electronics and electric power systems. Here, a new class of multilayer‐structured polymer nanocomposites with high energy and power densities is presented. The outer layers of the trilayered structure are composed of boron nitride nanosheets dispersed in poly(vinylidene fluoride) (PVDF) matrix to provide high breakdown strength, while PVDF with barium strontium titanate nanowires forms the central layer to offer high dielectric constant of the resulting composites. The influence of the filler contents on the electrical polarization, breakdown strength, and energy density is examined. Simulations are carried out to model the electrical tree formation in the layered nanocomposites and to verify the experimental breakdown results. The trilayered polymer nanocomposite with an optimized filler content displays a discharged energy density of 20.5 J cm^?3 at Weibull breakdown strength of 588 MV m^?1, which is among the highest discharged energy densities reported so far. Moreover, the nanocomposite exhibits a superior power density of 0.91 MW cm^?3, more than nine times that of the commercially available biaxially oriented polypropylene. The findings of this research provide a new design paradigm for high‐performance dielectric polymer nanocomposites.     

A Hybrid Material Approach Toward Solution‐Processable Dielectrics Exhibiting Enhanced Breakdown Strength and High Energy Density

The ever‐increasing demand for compact electronics and electrical power systems cannot be met with conventional dielectric materials with limited energy densities. Numerous efforts have been made to improve the energy densities of dielectrics by incorporating ceramic additives into polymer matrix. In spite of increased permittivities, thus‐fabricated polymer nanocomposites typically suffer from significantly decreased breakdown strengths, which preclude a substantial gain in energy density. Herein, organic–inorganic hybrids as a new class of dielectric materials are described, which are prepared from the covalent incorporation of tantalum species into ferroelectric polymers via in situ sol‐gel condensation. The solution‐processed hybrid with the optimal composition exhibits a Weibull breakdown strength of 505 MV m^?1 and a discharged energy density of 18 J cm^?3, which are more than 40% and 180%, respectively, greater than the pristine ferroelectric polymer. The superior performance is mainly ascribed to the deep traps created in the hybrids at the molecular level, which results in reduced electric conduction and lower remnant polarization. Simultaneously, the formation of the cross‐linked networks enhances the mechanical strengths of the hybrid films and thus hinders the occurrence of the electromechanical breakdown. This work opens up new opportunities to solution‐processed organic materials with high energy densities for capacitive electrical energy storage.     

Ultrahigh Energy Density of Antiferroelectric PbZrO3-Based Films at Low Electric Field

Dielectric capacitors play a vital role in advanced electronics and power systems as a medium of energy storage and conversion. Achieving ultrahigh energy density at low electric field/voltage, however, remains a challenge for insulating dielectric materials. Taking advantage of the phase transition in antiferroelectric (AFE) film PbZrO₃ (PZO), a small amount of isovalent (Sr²⁺) / aliovalent (La³⁺) dopants are introduced to form a hierarchical domain structure to increase the polarization and enhance the backward switching field E_A simultaneously, while maintaining a stable forward switching field E_F. An ultrahigh energy density of 50 J cm⁻³ is achieved for the nominal Pb_0.925La_0.05ZrO₃ (PLZ5) films at low electric fields of 1 MV cm⁻¹, exceeding the current dielectric energy storage films at similar electric field. This study opens a new avenue to enhance energy density of AFE materials at low field/voltage based on a gradient-relaxor AFE strategy, which has significant implications for the development of new dielectric materials that can operate at low field/voltage while still delivering high energy density.     

Highly Thermally Conductive Dielectric Nanocomposites with Synergistic Alignments of Graphene and Boron Nitride Nanosheets

Electrically insulating polymer dielectrics with high energy densities and excellent thermal conductivities are showing tremendous potential for dielectric energy storage. However, the practical application of polymer dielectrics often requires mutually exclusive multifunctional properties such as high dielectric constants, high breakdown strengths, and high thermal conductivities. The rational assembly of 2D nanofillers of boron nitride nanosheets (BNNS) and reduced graphene oxide (rGO) into a well‐aligned micro‐sandwich structure in polyimide (PI) composites is reported. The alternating stacking of rGO and BNNS synergistically exploits the large difference in their electrical conductivities to yield a high dielectric constant with a moderate breakdown strength. Moreover, the distinctively separated rGO and BNNS layers give rise to higher thermal conductivities of composites than those containing mixed fillers because of reduced phonon scattering at the interfaces between two identical fillers, as verified by molecular dynamics simulations. Consequently, the micro‐sandwich nanocomposite prevails over the PI film with a simultaneously high dielectric constant of ≈579, a high energy density (43‐fold higher than PI) and an excellent thermal conductivity (11‐fold higher than PI) at a low hybrid filler content of only 2.5 vol%. The multifunctional nanocomposites developed in this work are promising for flexible dielectrics with excellent heat dissipation.     

Maximizing the Energy Density of Dielectric Elastomer Generators Using Equi‐Biaxial Loading

Dielectric elastomer generators (DEGs) for harvesting electrical energy from mechanical work have been demonstrated but the energy densities achieved are still small compared with theoretical predictions. In this study, significant improvements in energy density (560 J/kg with a power density of 280 W/kg and an efficiency of 27%) are achieved using equi‐biaxial stretching, a mechanical loading configuration that maximizes the capacitance changes. The capacitance of dielectric elastomers subjected to equi‐biaxial stretches is demonstrated to be proportional to the fourth power of the stretch. Quantification of the individual energy contributions indicates that attaining higher conversion efficiencies is limited by viscous losses within the acrylic elastomer, suggesting that still higher conversion efficiencies with other elastomers should be attainable with our novel mechanical loading design.     

固体电介质中电偶极子热刺激电流与任意束缚能级分布谱

本文对单一束缚能级下电偶极子传统的热刺激电流，尤其是对其中超越函数积分物理意义加以分析后，首次导出了具有任意束缚能级的电偶极子热刺激电流理论，用假设的分布检验该结果表明近似解与精确解符合得相当好，应用本文的结果可以方便地确定对电流贡献的电偶极子数和束缚能级。     

2D Fillers Highly Boost the Discharge Energy Density of Polymer-Based Nanocomposites with Trilayered Architecture

A new class of trilayered architecture blends polymer-based nanocomposites with excellent discharge energy densities (U_dis) is presented. The preferable energy storage performance is achieved in sandwich structured nanocomposite (PIP) films. The outer polarization-layers (P-layer) of the PIP film are composed of Sr₂Nb₂O₇ nanosheets (SNONSs) as well as boron nitride nanosheets (BNNSs) dispersed in poly(vinylidene fluoride) (PVDF)/ polymethyl methacrylate (PMMA) blend polymer matrix (BPM) to provide high dielectric constant, while PVDF/PMMA with BNNSs forms the central insulation-layer (I-layer) to offer high dielectric breakdown strength (E_b) of the resulting nanocomposite films. The dielectric performance, Weibull breakdown strength, and energy storage capacity of single and multi-layer nanocomposites as a function of filler content are systematically examined. The evolution of electric trees is simulated via finite element methods to verify the experimental dielectric breakdown results in single layer nanocomposite films. The PIP film with optimized filler content displays a discharge energy density of 31.42 J cm⁻³ with a significantly improved charge–discharge efficiency of ≈71% near the Weibull breakdown strength of 655.16 MV m⁻¹, which is the highest among the polymer-based nanocomposites under the equivalent dielectric breakdown strength at present.     

High‐Performance Ferroelectric–Dielectric Multilayered Thin Films for Energy Storage Capacitors

Herein, the effect of the insertion of a thin dielectric HfO₂:Al₂O₃ (HAO) layer at different positions in the Pt/0.5Ba(Zr_0.2Ti_0.8)O₃–0.5(Ba_0.7Ca_0.3)TiO₃ (BCZT)/Au structure on the energy storage performance of the capacitors is investigated. A high storage performance is achieved through the insertion of a HAO layer between BCZT and Au layers. The insertion of the dielectric layer causes a depolarization field which results in a high linearity hysteresis loop with low energy dissipation. The Pt/BCZT/HAO/Au capacitors show an impressive energy storage density of 99.8 J cm^?3 and efficiency of 71.0%, at an applied electric field of 750 kV cm^?1. Further, no significant change in the energy storage properties is observed after passing 10⁸ switching cycles through the capacitor. The presence of resistive switching (RS) in leakage current characteristics confirms the strong charge coupling between ferroelectric and insulator layers. The same trend of the RS ratio and the energy storage performance with the variation of the architecture of the devices suggests that the energy storage properties can be improved through the charge coupling between the layers. By combining ferroelectrics and dielectrics into one single structure, the proposed strategy provides an efficient way for developing highly efficient energy storage capacitors.     

2D Antiferroelectric Hybrid Perovskite with a Large Breakdown Electric Field And Energy Storage Density

Energy conversion and storage devices are highly desirable for the sustainable development of human society. Hybrid organic–inorganic perovskites have shown great potential in energy conversion devices including solar cells and photodetectors. However, its potential in energy storage has seldom been explored. Here the crystal structure and electrical properties of the 2D hybrid perovskite (benzylammonium)₂PbBr₄ (PVK-Br) are investigated, and the consecutive ferroelectric-I (FE1) to ferroelectric-II (FE2) then to antiferroelectric (AFE) transitions that are driven by the orderly alignment of benzylamine and the distortion of [PbBr₆] octahedra are found. Furthermore, accompanied by field-induced AFE to FE transition near room temperature, a large energy storage density of ≈1.7 J cm⁻³ and a wide working temperature span of ≈70 K are obtained; both of which are among the best in hybrid AFEs. This good energy storage performance is attributed to the large polarization of ≈7.6 µC cm⁻² and the high maximum electric field of over 1000 kV cm⁻¹, which, as revealed by theoretical calculations, originate from the cooperative coupling between the [PbBr₆] octahedral framework and the benzylamine molecules. The research clarifies the discrepancy in the phase transition character of PVK-Br and shed light on developing high-performance energy storage devices based on 2D hybrid perovskite.     

Superior High-Temperature Energy Density in Molecular Semiconductor/Polymer All-Organic Composites

High-temperature dielectric polymers are in constant demand for the multitude of high-power electronic devices employed in hybrid vehicles, grid-connected photovoltaic and wind power generation, to name a few. There is still a lack, however, of dielectric polymers that can work at high temperature (> 150 °C). Herein, a series of all-organic dielectric polymer composites have been fabricated by blending the n-type molecular semiconductor 1,4,5,8-naphthalenetetracarboxylic dianhydride (NTCDA) with polyetherimide (PEI). Electron traps are created by the introduction of trace amounts of n-type small molecule semiconductor NTCDA into PEI, which effectively reduces the leakage current and improves the breakdown strength and energy storage properties of the composite at high temperature. Especially, excellent energy storage performance is achieved in 0.5 vol.% NTCDA/PEI at the high temperatures of 150 and 200 °C, e.g., ultrahigh discharge energy density of 5.1 J cm⁻³ at 150 °C and 3.2 J cm⁻³ at 200 °C with high discharge efficiency of 85–90%, which is superior to its state-of-the-art counterparts. This study provides a facile and effective strategy for the design of high-temperature dielectric polymers for advanced electronic and electrical systems.     

一种可集成高密度氮氧化硅介质工艺

针对传统二氧化硅、氮化硅等介质材料在制作MOS电容时存在电容密度低、界面特性差的问题,通过对氮离子注入、氮硅氧化实验的分析,成功开发出一种采用注入氮并氧化制作氮氧化硅介质材料的工艺;并使用该工艺研制出与36 V双极工艺兼容、介质的相对介电常数为5.51、击穿电压达81 V、电容密度为0.394 fF/μm²的高密度MOS电容,较传统可集成二氧化硅/氮化硅复合介质电容的电容密度提高了35.86%。该工艺还可用于制作大功率MOSFET的栅介质,可提高器件的可靠性。     

Van der Waals Epitaxy Enables Rollable Dielectric Superlattice for Record High Overall Energy Density

Nanoengineered polar oxide films have attracted much attention for electric energy storage thanks to their high energy density, though they are all deposited on thick and rigid substrates, resulting in inferior overall energy density and poor manufacturability. Herein, an alternative strategy is developed for oxide dielectrics utilizing van der Waals epitaxy on ultrathin and flexible mica substrate, with a dielectric superlattice of Pb_0.92La_0.08(Zr_0.95Ti_0.05)O₃-SrTiO₃ carefully engineered to break its long-range antiferroelectric polar order. An ultrathin flexible capacitor is obtained as a result, with a record high overall energy density of 12.19 J cm⁻³ and an efficiency of 90.98%, and there is much room for further improvement since mica substrate can approach 2D limit. The superlattice can be easily rolled for large-scale manufacturing, and the energy storage performances are well maintained under large bending deformation as well as extended bending cycling. The study thus establishes a viable route for dielectric oxide films, paving way for their practical applications in high-energy density capacitors.     

Energy Efficiency Based on Joint Data Packet Fragmentation and Cooperative Transmission

Energy efficiency （EE） is a key requirement for the design of short-range communication network. In order to alleviate energy consumption （EC） constraint, a novel layered heterogeneous mobile cloud architecture is proposed in this paper. Based on the proposed layered heterogeneous mobile cloud architecture, we establish an appropriate energy consumption model, and design an energy efficiency scheme based on joint data packet fragmentation and cooperative transmission and analyze the energy efficiency corresponding to different packet sizes and the cloud size. Simulation results show that, when all nodes of the cloud are accessing the same size of data packet fragmentation, the proposed layered heterogeneous mobile cloud architecture can provide significant energy savings. The results provide useful insights into the possible operation of the strategies and show that significant energy consumption reductions are possible.