operate concurrently under high electric fields and elevated temperatures approaching or surpassing 150 °C. [2,4,8,[11][12][13] However, to date, the search for polymer dielectrics that provide appreciable energy densities at temperatures well above 100 °C has led to only marginal success. High temperature operation under high electric field is challenging for polymer dielectrics. For example, biaxially oriented polypropylene (BOPP), the state-of-the-art commercially available dielectric polymer used for energy storage, has a remarkable breakdown strength of ≈700 MV m −1 and ultralow loss, but can only operate continuously at temperatures up to 85 °C and for a short duration with significant derating at 105 °C. [14,15] Many heat resistant polymers have been designed and studied for high-temperature applications, but they are incapable of operating at an electric field similar to BOPP. [11,16,17] This is because their conjugated aromatic backbones that are able to withstand high temperature, built at the cost of largely reduced bandgaps, lead to high electrical conductivities and poor energy densities especially at elevated temperatures. Recent efforts for enhanced energy storage performance at high temperature via nanocomposites or coating modifications of polymer films, although encouraging, are prohibitively challenging for industrial-scale production due to requirements of (either) materials cost and (or) laborious multi-step synthesis and processing. [2,12,13,18,19] As a result, BOPP is still used today with cumbersome active cooling. The availability of flexible polymer dielectrics, capable of stable operation under ultrahigh electric field and elevated temperature is the limiting factor for high power density electrification and electronics.Due to hot carrier excitation, injection, and transport, assisted under thermal and electric extremes, polymers exhibit a nonlinear increase in electrical conduction, [20][21][22] leading to the reduction of the discharged energy density, largely increased energy loss and ultimately dielectric breakdown failure [23] . While the complexity of these processes makes the study of engineering conduction mechanism under critical electric fields far from fully understood, past studies revealed the dominant role of the bandgap in determining electrical conduction and intrinsic breakdown strength of the polymer dielectrics. [20,[24][25][26][27] However, careful evaluation of common high-temperature polymers reveals, unfortunately, an inverse Flexible dielectrics operable under simultaneous electric and thermal extremes are critical to advanced electronics for ultrahigh densities and/or harsh conditions. However, conventional high-performance polymer dielectrics generally have conjugated aromatic backbones, leading to limited bandgaps and hence high conduction loss and poor energy densities, especially at elevated temperatures. A polyoxafluoronorbornene is reported, which has a key design feature in that it is a polyolefin consisting of repeating units of fairly rigid fused bicycl...

The dielectric constant (ϵ) is a critical parameter utilized in the design of polymeric dielectrics for energy storage capacitors, microelectronic devices, and high-voltage insulations. However, agile discovery of polymer dielectrics with desirable ϵ remains a challenge, especially for high-energy, high-temperature applications. To aid accelerated polymer dielectrics discovery, we have developed a machine-learning (ML)-based model to instantly and accurately predict the frequency-dependent ϵ of polymers with the frequency range spanning 15 orders of magnitude. Our model is trained using a dataset of 1210 experimentally measured ϵ values at different frequencies, an advanced polymer fingerprinting scheme and the Gaussian process regression algorithm. The developed ML model is utilized to predict the ϵ of synthesizable 11,000 candidate polymers across the frequency range 60–1015 Hz, with the correct inverse ϵ vs. frequency trend recovered throughout. Furthermore, using ϵ and another previously studied key design property (glass transition temperature, Tg) as screening criteria, we propose five representative polymers with desired ϵ and Tg for capacitors and microelectronic applications. This work demonstrates the use of surrogate ML models to successfully and rapidly discover polymers satisfying single or multiple property requirements for specific applications.

A paradigm-shifting design strategy is demonstrated that unifies the treatment of electronic and conformational properties of polymer dielectrics for concurrent high electric field and elevated temperature harsh conditions.

The electronic structures of carbon nanotube/RuO2 core/shell nanocomposite (RuO2 thin layer coated multiwalled carbon nanotubes (MWNTs)) have been studied by X-ray absorption near-edge structures (XANES) at C K-edge, O K-edge, and Ru M5,4- and L3-edges. The variation in white-line features of the XANES at these edges supports strongly that RuO2 interacts with MWNTs through Ru−O−C bonding, which also results in charge redistribution between C 2p-derived states in MWNT and the conduction band in RuO2. Such chemical bonding is necessary to immobilize RuO2 on MWNT and ensures good conductivity of MWNT/RuO2 core/shell nanocomposite.

The organic insulator–metal interface is the most important junction in flexible electronics. The strong band offset of organic insulators over the Fermi level of electrodes should theoretically impart a sufficient impediment for charge injection known as the Schottky barrier. However, defect formation through Anderson localization due to topological disorder in polymers leads to reduced barriers and hence cumbersome devices. A facile nanocoating comprising hundreds of highly oriented organic/inorganic alternating nanolayers is self‐coassembled on the surface of polymer films to revive the Schottky barrier. Carrier injection over the enhanced barrier is further shunted by anisotropic 2D conduction. This new interface engineering strategy allows a significant elevation of the operating field for organic insulators by 45% and a 7× improvement in discharge efficiency for Kapton at 150 °C. This superior 2D nanocoating thus provides a defect‐tolerant approach for effective reviving of the Schottky barrier, one century after its discovery, broadly applicable for flexible electronics.

The dielectric constant of polymers was increased by combining flexible segments and rigid polar segments in the polymer backbone.

No abstract

Due to their electrically polarized air‐filled internal pores, optimized ferroelectrets exhibit a remarkable piezoelectric response, making them suitable for energy harvesting. Expanded polytetrafluoroethylene (ePTFE) ferroelectret films are laminated with two fluorinated‐ethylene‐propylene (FEP) copolymer films and internally polarized by corona discharge. Poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS)‐coated spandex fabric is employed for the electrodes to assemble an all‐organic ferroelectret nanogenerator (FENG). The outer electret‐plus‐electrode double layers form active device layers with deformable electric dipoles that strongly contribute to the overall piezoelectric response in the proposed concept of wearable nanogenerators. Thus, the FENG with spandex electrodes generates a short‐circuit current which is twice as high as that with aluminum electrodes. The stacking sequence spandex/FEP/ePTFE/FEP/ePTFE/FEP/spandex with an average pore size of 3 µm in the ePTFE films yields the best overall performance, which is also demonstrated by the displacement‐versus‐electric‐field loop results. The all‐organic FENGs are stable up to 90 °C and still perform well 9 months after being polarized. An optimized FENG makes three light emitting diodes (LEDs) blink twice with the energy generated during a single footstep. The new all‐organic FENG can thus continuously power wearable electronic devices and is easily integrated, for example, with clothing, other textiles, or shoe insoles.