Fabrication of High Thermal Conductivity Nanodiamond/Aramid Nanofiber Composite Films with Superior Multifunctional Properties.

Polymer-based thermally conductive materials are preferred for heat dissipation owing to their low density, flexibility, low cost, and easy processing. Researchers have been trying to develop a polymer-based composite film with excellent thermal conductivity (TC), mechanical strength, thermal stability, and electrical properties. However, synergistically achieving these properties in a single material is still a challenge. To address the above requirements, we prepared poly(diallyldimethylammonium chloride)-functionalized nanodiamond (ND@PDDA)/aramid nanofiber (ANF) composite films using a self-assembly strategy. Owing to a strong interfacial interaction arising from electrostatic attraction, ND particles attract strongly along the ANF axis to form ANF/ND "core-sheath" arrangements. These assemblies self-construct three-dimensional thermally conductive networks through ANF gelation precipitation, which was analyzed as the key parameter for the realization of high thermal performances. The as-prepared ND@PDDA/ANF composite films exhibited high in-plane and through-plane TCs up to 30.99 and 6.34 W/m·K, respectively, at a 50 wt % functionalized ND loading, representing the optimal values among all previously reported polymer-based electrical insulating composite films. Furthermore, the nanocomposites also achieved other properties necessary for realistic applications, such as outstanding mechanical properties, excellent thermal stability, ultra-low thermal expansion coefficient, excellent electrical insulation, low dielectric constant, low dielectric loss, and outstanding flame retardancy. Thus, this excellent comprehensive performance enables the ND@PDDA/ANF composite films to be used as advanced multifunctional nanocomposites in thermal management, flexible electronics, and intelligent wearable equipment.