Thermal-conductive yet electrical-insulating polymer composites with outstanding mechanical properties have attracted increasing attention in the electronic field. Herein, three-dimensional (3D) thermal-conductive networks were built in PVDF matrix via electrostatic repulsion of positively charged hexagonal boron nitride (m-hBN) and bridging of silica-coated carbon nanotubes (MWCNTs-SiO₂). The results indicated that 25 wt% m-hBN/MWCNTs-SiO₂/PVDF presented fascinating characteristics: a high thermal conductivity of 1.51 W/(m·K) and an excellent tensile strength of 55.02 MPa, with the enhancements of 586% and 25% respectively compared to pure PVDF; besides, superior dielectric properties and electrical insulation were obtained, with dielectric constant of 4.95, dielectric loss tangent of 0.14 at 1 MHz, and volume resistivity of 3.45 × 10¹² Ω·cm. The Effective Medium Approximation (EMA) model revealed that the formation of 3D-networks could significantly decrease thermal resistance and promote phonon transmission. The outstanding heat dissipation capability of m-hBN/MWCNTs-SiO₂/PVDF was verified by infrared imaging test, indicating its potential applications for thermal management.

具有优异机械性能的导热但电绝缘的聚合物复合材料在电子领域引起了越来越多的关注。在此，通过带正电的六方氮化硼（m-hBN）的静电排斥作用和桥接二氧化硅涂层的碳纳米管（MWCNTs-SiO ₂），在PVDF矩阵中建立了三维（3D）导热网络。结果表明，m-hBN / MWCNTs-SiO _2为25 wt％/ PVDF具有令人着迷的特性：1.51 W /（m·K）的高导热系数和55.02 MPa的优异拉伸强度，与纯PVDF相比分别提高了586％和25％；除此之外，获得了优异的介电性能和电绝缘，具有4.95的介电常数，在1MHz的0.14介质损耗角正切，和3.45×10的体积电阻率¹² Ω·cm以下。有效介质近似（EMA）模型显示3D网络的形成可以显着降低热阻并促进声子传输。m-hBN / MWCNTs-SiO ₂ / PVDF的出色散热性能通过红外成像测试得到验证，表明其在热管理方面的潜在应用。