Sun Liang, Zhang Fengyuan, Li Li, Liang Jiajie, Dong Jiufeng, Pan Zizhao, Niu Yujuan, Chen Jiaxin, Liu Yuqi, Lu Yani, Wu Kai, Li Qi, Li Jiangyu, Wang Qing, Wang Hong
Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen, Guangdong, 518055, China.
Department of Materials Science and Engineering, The Pennsylvania State University, University Park, Pennsylvania, 16802, USA.
Adv Mater. 2025 Jan;37(3):e2412561. doi: 10.1002/adma.202412561. Epub 2024 Dec 2.
Polymer dielectrics are essential for advanced electronics and electrical power systems, yet they suffer from low energy density (U) due to their low dielectric constant (K) and the inverse relationship between K and breakdown stength (E). Here a scalable approach utilizing the designed molecularly interpenetrating interfaces is presented to achieve all-organic dielectric polymers with high U and charge-dischage efficiency (η). Distinctive intermolecular interactions and microstructural changes, as demonstrated experimentally and theoretically, are introduced by the molecularly interpenetrating interfaces, resulting in simultaneous improvements in dielectric responses and mechanical strength while inhibiting electrical conduction - outcomes unattainable in conventional layered polymers. Consequently, exceptional improvments in both K and E are achieved, yielding a very high U of 22.89 J cm with η ≥ 90%, outperforming current layered polymer dielectrics. The bilayers can be easily fabricated into large-area films with high uniformity and outstanding capacitive stability (>500 000 cycles), offering a practical route to scalable high-U polymer dielectrics for electrical energy storage.
聚合物电介质对于先进电子和电力系统至关重要，但由于其低介电常数（K）以及K与击穿强度（E）之间的反比关系，它们的能量密度（U）较低。本文提出了一种利用设计的分子互穿界面的可扩展方法，以实现具有高U和充放电效率（η）的全有机介电聚合物。实验和理论表明，分子互穿界面引入了独特的分子间相互作用和微观结构变化，从而在抑制导电的同时，实现了介电响应和机械强度的同步提高，这是传统层状聚合物无法实现的结果。因此，K和E都得到了显著提高，产生了22.89 J/cm³的非常高的U，η≥90%，优于目前的层状聚合物电介质。这些双层膜可以很容易地制成具有高均匀性和出色电容稳定性（>500 000次循环）的大面积薄膜，为用于电能存储的可扩展高U聚合物电介质提供了一条实用途径。
