Design of efficient thermal conductive epoxy resin composites via highspeed transport pathways of heterogeneous compatible carbon framework

Thermal interface materials are crucial for addressing the hot issues of a rapid increase in thermal density in narrow and limited service spaces. Flexible and designable epoxy resin (EP) based composites are competitive choice yet lacks desirable thermal conductivity (∼0.2 W m −1  K −1 ) and mechanical properties (tensile strength: ∼19.6 MPa). Herein, EP-based composites with a reinforced three-dimensional (3D) interconnected carbon material architecture were prepared by in-situ growing 1D carbon nanotubes (CNTs) on the surface of 2D carbon fiber braid (CFB) and infiltrating matrix EP. CNTs not only promote the wettability between carbon fibers inside CFB and EP but also observably bridge the adjacent carbon fibers. The analysis of numerical models reveals the prominent contribution of 3D CFB/CNTs network to a significant increase in thermal conductivity. Non-equilibrium molecular dynamics (NEMD) indicates the high intrinsic thermal conductivity of CNTs in both systems: single CNT model and CNT/Ni model. The coupling behavior of high-frequency phonons at the interface contributes to the in-plane thermal transport. The in-plane thermal conductivity of 7.86 W m −1  K −1 and the through-plane thermal conductivity of 5.85 W m −1  K −1 are obtained in the composites with 23.2 wt% hybrid fillers, increased by 3830 % compared to neat EP. The tensile (58.93 MPa) and compressive strength (138.83 MPa) are also enhanced, meeting practical demands. These properties even perform no obvious changes after 100 cycles of bending. The stable and reliable EP-based composites with outstanding comprehensive performance designed by this work have enormous application potential in the advanced heat dissipation system.