Honeycomb networks of boron nitride/nanodiamond with interlocking interfaces enhance the application reliability of silicone rubber thermal conductivity composites

Abstract The three‐dimensional (3D) boron nitride (BN) thermal conductive networks, crafted through layer‐by‐layer assembly, hold tremendous potential for the development of insulating thermal interface materials (TIMs) with exceptional thermal conductivity. Nevertheless, maintaining the thermal conductive stability of this structure type during application remains a considerable challenge. Herein, initially, the honeycomb networks of boron nitride/nanodiamond (ND/kBN) with interlocking interfaces were prepared by electrostatic self‐assembly and ice template method. Subsequently, thermal conductivity composites of flexible silicone rubber (VQM) were acquired through vacuum‐assisted infiltration. The composites demonstrated improved through‐plane thermal conductivity with 1.03 W/(m K) at a 9.9 vol% content of ND/kBN while exhibiting relatively ideal dielectric properties. More importantly, the thermal conductive properties of the composites still maintain at 96.1% and 91.9%, respectively, even after undergoing 30% compressive deformation for 1 h and being bent 300 times. This study presents a novel strategy that not only improves the thermal conductivity of composites but also ensures the reliability of their applications. Highlights Nanodiamond (ND) is anchored onto the kBN surface by electrostatic self‐assembly. ND/kBN filler honeycomb network with an interlocking interface was prepared. Flexible composites with high thermal conductivity (TC) were prepared. The composites exhibit excellent TC stability after experiencing deformation.