Polymer-based dielectric composites are potential substitute dielectrics for organic thin film capacitors. In this work, the exfoliated molybdenum disulfide (MoS₂) was functionalized by mussel-inspired poly(dopamine) (PDA) to form core-shell structured composites (MoS₂@PDA) under easy-handling and eco-friendly conditions, and then as filler incorporated into poly(arylene ether nitrile) (PEN) matrix. The interfacial interaction and dispersion of MoS₂@PDA in PEN matrix were improved by the strong adhesion of PDA interlayer to exfoliated MoS₂, π-π conjugation and hydrogen bond interactions, which formed by the polar nitrile group of PEN and catechol groups of PDA. Therefore, the PEN/MoS₂@PDA composite films exhibited enhanced dielectric constant, synchronously maintaining better flexibility, thermal stability and the same level of dielectric loss with PEN. Particularly, the addition of 20 wt% MoS₂@PDA into PEN matrix leaded to substantial growth of dielectric constant up to 12.9 at 1 kHz, while the PEN matrix was just 4.2. Meanwhile, the dielectric composites maintained relatively low dielectric loss of 0.022 at 1 kHz, which was ascribed to the improved compatibility and interfacial interaction between filler and PEN. All in all, a eco-friendly and easy-handling strategy was provided to tune the dielectric constant and dielectric loss of semiconductor/polymer composites, which has great potential to promote the development of dielectric in the fields of organic thin film capacitors.

聚合物基电介质复合材料是有机薄膜电容器的潜在替代电介质。在这项工作中，剥离的二硫化钼（MoS ₂）被贻贝启发的聚（多巴胺）（PDA）功能化，在易于处理和环保的条件下形成核壳结构复合材料（MoS ₂ @PDA），然后作为填料掺入聚（亚芳基醚腈）（PEN）基质中。通过PDA中间层与剥离的MoS ₂的强粘附、π-π共轭和氢键相互作用，PEN的极性腈基团和PDA的邻苯二酚基团形成了MoS ₂ @PDA在PEN基质中的界面相互作用和分散性. 因此，PEN/MoS ₂@PDA 复合薄膜表现出更高的介电常数，同时保持更好的柔韧性、热稳定性和与 PEN 相同水平的介电损耗。特别是，在PEN 基质中添加 20 wt% MoS ₂ @PDA 导致介电常数在 1 kHz 下大幅增长至 12.9，而 PEN 基质仅为 4.2。同时，介电复合材料在 1 kHz 时保持相对较低的介电损耗为 0.022，这归因于填料与 PEN 之间的相容性和界面相互作用的改善。总之，提供了一种环保且易于操作的策略来调节半导体/聚合物复合材料的介电常数和介电损耗，这对促进有机薄膜电容器领域电介质的发展具有巨大潜力。