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Polymer dielectrics are key components for electrostatic capacitors in energy, transportation, military, and aerospace fields, where their operation temperature can be boosted beyond 125 °C. While most polymers bear poor thermal stability and severe dielectric loss at elevated temperatures, numerous linear polymers with linear D-E loops and low dielectric permittivity exhibit low loss and high thermal stability. Therefore, the broad prospect of electrostatic capacitors under extreme conditions is anticipated for linear polymers, along with intensive efforts to enhance their energy density with high efficiency in recent years. In this article, an overview of recent progress in linear polymers and their composites for high-energy-density electrostatic capacitors at elevated temperatures is presented. Three key factors determining energy storage performance, including polarization, breakdown strength, and thermal stability, and their couplings are discussed. Strategies including chain modulation, filler selection, and design of topological structure are summarized. Key parameters for electrical and thermal evaluations of polymer dielectrics are also introduced. At the end of this review, research challenges and future opportunities for better performance and industrialization of dielectrics based on linear polymers are concluded.

Emerging dielectric composites consisting of polymer and ceramic nano-inclusions or several polymers facilitate the development of capacitive energy storage materials, as they can preserve high breakdown strength and exhibit enhanced dielectric constant. Ferroelectric poly(vinylidene fluoride) (PVDF) and its copolymers have been intensively studied as the matrices because of their high intrinsic dielectric constant and breakdown strength. Here, we review the recent advances on improving the energy density of PVDF-based composite dielectrics. It is concluded that, promotion of energy density is mainly established on enhanced breakdown strength and improved discharge efficiency. The microstructure design, material performance, and mechanism associated with these parameters are described. Perspectives for future development on PVDF-based nanocomposites and application of other potential polymer matrices are presented at last.

High-energy-density dielectric materials are highly desirable for the miniaturization and integration of modern electronics and power modules for applications in electrical power, communication, medical and defense systems. However, the conventional polymer nanocomposites with nanofillers randomly dispersed exhibit a limited energy storage performance (e.g. discharged energy density

Poly(vinylidene fluoride) (PVDF)-based dielectric polymers are in great demand for the future electronic and electrical industry because of their high dielectric constants and energy density. However, some issues that limit their practical applications remain unsolved. One of the most urgent issues is their high dielectric loss and hence low efficiency. In this contribution, we proposed and demonstrate that substantially enhanced discharge efficiency of PVDF-based polymers nanocomposites could be achieved by simultaneously optimizing their topological-structure and phase composition. In the poly(vinylidene fluoride-co-hexafluoropropylene) (P(VDF-HFP))/poly(vinylidene fluoride-ter-trifluoroethylene-ter-chlorofluoroethylene) (P(VDF-TrFE-CFE)) multilayered nanocomposites fabricated by non-equilibrium process, an ultrahigh discharge efficiency of ~85% is achieved up to 600 MV/m, which is the highest discharge efficiency reported so far for any polar-polymer dielectric materials at such high electric field. By adjusting the quenching temperature, the phase-composition hence dielectric permittivity in the terpolymer layers could be tuned for suppressed ferroelectric loss. Results of phase-field simulations further reveal that local electric field is substantially weakened at the interfaces between the Co/Ter polymer layers, which will act as barriers to motion of charge carriers and give rise to much suppressed conduction loss and a remarkably enhanced breakdown strength. Synergy of the optimized topological-structure and phase-composition thus leads to a nanocomposite that exhibits an unprecedented high discharge efficiency of the multilayered nanocomposites that is comparable to the bench-mark biaxially oriented polypropylene (BOPP) at high electric field as well as a high discharge energy density that is over 10 times higher than that of BOPP.

Multiplexing physical dimensions to realize multidimensional storage in a single material has been a goal to increase storage density and data security. Multidimensional storage is only achieved in optical storage material (OSM) by far. Poly(vinylidene fluoride) (PVDF), a semicrystalline polymer, is widely studied as a candidate for ferroelectric random access (FeRAM). Herein, the atomic force microscopy (AFM)-based infrared spectroscopy techniqueis used to induce multilevel phase transformations in PVDF ultrathin film on nanometric scales and for writing/readout of IR signals. An optical/ferroelectric multiplexing PVDF memory, where information can be coded with independent four-level optical IR and bilevel ferroelectric signals, is demonstrated. High data security and a storage density up to 180 GBit in.

Ferroelectric memories are endowed with high data storage density by nanostructure designing, while the robustness is also impaired. For organic ferroelectrics favored by flexible memories, low Curie transition temperature limits their thermal stability. Herein, a ferroelectric random access memory (FeRAM) is demonstrated based on an array of P(VDF‐TrFE) lamellae by self‐assembly. Written data shows enhanced thermal endurance up to 90 °C and undergoes 12 thermal cycles between 30 and 80 °C with little volatilization. The promoted thermal stability is attributed to pinning effect at interfaces between grain boundaries and lamellae, where charged domain walls and charged defects are coupled. These results provide a strategy for improving robustness of organic flexible FeRAMs, and reveal an attracting coupling effect between different phases of ferroelectric polymer.