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Machine learning has shown its great potential in the accelerated discovery of advanced materials in the field of computational molecular design. High-temperature polymer dielectrics are urgently required with the emerging applications of energy-storage dielectric film capacitors under high-temperature conditions. Here, we demonstrate the successful prediction of polymers with a high dielectric constant (ɛ) and high glass transition temperature (Tg) using a Bayesian molecular design model. The model is trained on a joint data set containing 382 computed ɛ values using density functional perturbation theory and experimentally measured Tg values of ∼7000 polymers to build relative quantitative structure–property relationships and identify the promising polymers with specific desired range of dielectric constant and glass transition temperature. From the hypothetical polymer candidates, ten promising polymers are proposed based on their predicted properties and synthetic accessibility score for high-temperature dielectric film capacitors' application. Moreover, 250k novel polymer structures are generated with the model to support future polymer informatics research. This work contributes to the successful prediction of high-temperature polymer dielectrics using machine learning models. [ABSTRACT FROM AUTHOR]

Polymer composites with high energy density have been of great interest to scientists for a long time, and this accounts for a great wealth of experimental data that are available for interpretation. One of the important phenomena is the variation rate of the permittivity of composites, which always deviates from the linear increase and rises steeply toward the high concentration. Interestingly, the critical transition concentration is always located in the range of 20 vol. %–25 vol. %, but still far less than the common percolation threshold of composites. Through the analysis of the local electric field distribution and surface polarized charges distribution, the phenomenon is successfully interpreted as the effect of the electrostatic interactions between the adjacent polarized particles. Two specified composite configurations (BCC and FCC) are designed, and their dielectric properties have been systematically studied with the help of the finite element method and the phase field method. The simulation results indicate that the strength of the particles' interaction is short-range effective and depends closely on the gap distance between adjacent particles. When the gap distance is smaller than 0.8 times the radius of the particles, which is tantamount to the concentration larger than 20 vol. % and 25 vol. % for BCC and FCC, respectively, the electrostatic interaction of the particles is rather significant, resulting in an additional contribution on the variation of the dielectric properties of composites and vice versa. The synchronous variation tendency between the simulation results and experimental measurements demonstrates the effect of electrostatic interaction on the dielectric properties of composites. [ABSTRACT FROM AUTHOR]

Polymer‐based dielectrics with fast electrostatic energy storage and release, are crucial for advanced electronics and power systems. However, the deterioration of insulation performance and charge–discharge efficiency of polymer dielectrics at elevated temperatures and high electric fields hinder the applications of capacitors in harsh environments. Herein, a facile and scalable approach is reported to fabricating flexible high‐temperature polymer dielectrics for high‐efficiency energy storage by ultraviolet irradiation. The resultant dielectric films exhibit an augment of 493% in energy density and exceeding 800% in discharge efficiency at 200 °C (3.2 J cm−3 and over 90% discharge efficiency at 480 M V−1m for irradiated polyetherimide (PEI), 0.54 J cm−3, and below 10% discharge efficiency at 400 MV m−1 for pristine PEI) and excellent cycle performance. The injected space charge is found to be the dominant contributor to energy loss during the charge–discharge process. Free radicals introduced by ultraviolet irradiation can act as deep traps to capture injected charge and suppress space charge migration. This work clarifies the contribution of space charge to energy loss and demonstrates the effectiveness of ultraviolet irradiation in improving the capacitive performance of high‐temperature polymer dielectrics. These findings provide a novel paradigm for the rational design of high‐temperature polymer dielectrics for high‐efficiency energy storage. [ABSTRACT FROM AUTHOR]

With the development of advanced electronic devices and electric power systems, polymer-based dielectric film capacitors with high energy storage capability have become particularly important. Compared with polymer nanocomposites with widespread attention, all-organic polymers are fundamental and have been proven to be more effective choices in the process of scalable, continuous, and large-scale industrial production, leading to many dielectric and energy storage applications. In the past decade, efforts have intensified in this field with great progress in newly discovered dielectric polymers, fundamental production technologies, and extension toward emerging computational strategies. This review summarizes the recent progress in the field of energy storage based on conventional as well as heat-resistant all-organic polymer materials with the focus on strategies to enhance the dielectric properties and energy storage performances. The key parameters of all-organic polymers, such as dielectric constant, dielectric loss, breakdown strength, energy density, and charge-discharge efficiency, have been thoroughly studied. In addition, the applications of computer-aided calculation including density functional theory, machine learning, and materials genome in rational design and performance prediction of polymer dielectrics are reviewed in detail. Based on a comprehensive understanding of recent developments, guidelines and prospects for the future development of all-organic polymer materials with dielectric and energy storage applications are proposed.