Polymer-based composites with high dielectric constant and low loss are highly desirable due to their inherent advantages of easy processability, flexibility, and lightweight. Herein, a functional nanofillers, halloysite nanotubes (HNTs) decorated reduced graphene oxide (rGO) hybrid microstructures (HNTs@rGO) was successfully prepared via controllable electrostatic self-assembly and in-situ heat reduction method. These hybrid microstructures combine characteristics of natural 1D ceramic nanotubes with large aspect ratio and high electric conductivity of rGO micro-sheets, which provided ideal material collocation in the construction of microcapacitors. The HNTs not only effectively prevented direct contact between the rGO micro-sheets in the composites but also played an important role in forming dielectric interface within microcapacitors. Consequently, an HNTs@rGO/polyvinyl butyral (PVB) composites containing a very low content of 5 wt% rGO exhibited an ultra-high dielectric constant of 150 and an extremely low loss of 0.12 at 10³ Hz. It is believed that the unique characteristics and facile fabrication process of HNTs@rGO/PVB composite make it a potentially excellent candidate for flexible polymer-based dielectric materials applied in the capacitor fields.

具有高介电常数和低损耗的基于聚合物的复合材料由于其固有的容易加工性，柔韧性和轻质性的优点而非常令人期望。在此，通过可控的静电自组装和原位热还原法成功地制备了功能性纳米填料，埃洛石纳米管（HNTs）装饰的还原氧化石墨烯（rGO）杂化微结构（HNTs @ rGO）。这些混合微结构结合了天然一维陶瓷纳米管的特性，具有高长宽比和高导电率的rGO微片，为微电容器的构造提供了理想的材料搭配。HNTs不仅有效地防止了复合材料中rGO微片之间的直接接触，而且在微电容器内形成介电界面方面发挥了重要作用。³赫兹 据信，HNTs @ rGO / PVB复合材料的独特特性和简便的制造工艺使其成为电容器领域应用的基于柔性聚合物的介电材料的潜在优秀候选者。