As core components in electric/electronic fields, dielectric materials have recently received ever‐increasing interests. Among them, polymer‐based dielectric composites have drawn ever‐increasing attentions due to their high‐temperature resistance and excellent processibility. However, state‐of‐art studies mostly focus on the modification of single‐phase filler, while the heterogeneous three phase interactions between fillers and polymer matrix are rarely studied. To fill this gap, in this study, a novel strategy of interfacial design and structural construction of three‐phase BaTiO3/rGO/polymer nanocomposites have been promoted to simultaneously build interfacial barriers between adjacent rGO nanosheets and to enhance the interfacial polarization of rGO nanosheets for improved dielectric, thermal and mechanical properties. The dielectric constant of 0.6 wt% BT/ARGO/PEI reached 644@1 kHz with a dielectric loss of only 0.218, while these values for 0.5 wt% ARGO/PEI composites are 471 and 0.489, respectively. Meanwhile, the breakdown strength almost doubled (from 48 kV·mm−1 to 87 kV·mm−1) upon the addition of BaTiO3 (BT) nanoparticles. Moreover, the introduced BT nanoparticles significantly enhanced the intermolecular frictions between different materials and contributed largely to promoted mechanical and thermal properties. We therefore speculate this work establishes a strong foundation for fabricating three heterogeneous‐phase high dielectric polymer materials with excellent dielectric, thermal and mechanical properties.Highlights Graphene oxide was modified by APTES and reduced by L‐Ascorbic Acid. Three‐phase BT/ARGO/PEI composites showed enhanced dielectric properties. The incorporated BT nanoparticles reduced the dielectric loss. The thermal and mechanical properties of BT/ARGO/PEI composites are optimized. Interfacial interactions between different phase of materials are studied.

中文翻译：

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BaTiO3/rGO/聚醚酰亚胺复合材料的三相界面设计可增强介电、热和机械性能

作为电气/电子领域的核心部件，介电材料近年来受到越来越多的关注。其中，聚合物基介电复合材料因其耐高温和优异的加工性能而受到越来越多的关注。然而，最新的研究主要集中在单相填料的改性上，而很少研究填料与聚合物基体之间的非均相三相相互作用。为了填补这一空白，在本研究中，三相 BaTiO 的界面设计和结构构建的新策略3/rGO/聚合物纳米复合材料已被推广用于同时在相邻rGO纳米片之间建立界面屏障，并增强rGO纳米片的界面极化，以改善介电、热和机械性能。 0.6 wt% BT/ARGO/PEI 的介电常数达到 644@1 kHz，介电损耗仅为 0.218，而 0.5 wt% ARGO/PEI 复合材料的介电常数分别为 471 和 0.489。同时，击穿强度几乎翻倍（从 48 kV·mm−1至 87 kV·mm−1）添加BaTiO后3（BT）纳米颗粒。此外，引入的BT纳米粒子显着增强了不同材料之间的分子间摩擦，并在很大程度上促进了机械和热性能的提高。因此，我们推测这项工作为制造具有优异介电、热和机械性能的三种异相高介电聚合物材料奠定了坚实的基础。 氧化石墨烯经过 APTES 改性并被 L-抗坏血酸还原。 三相 BT/ARGO/PEI 复合材料表现出增强的介电性能。 掺入的 BT 纳米粒子降低了介电损耗。 BT/ARGO/PEI 复合材料的热性能和机械性能得到优化。 研究不同相材料之间的界面相互作用。