Preparation and Thermal Conductivity of Epoxy Composites Cured by Imine‐Functionalized <scp>PDMS</scp>

ABSTRACT With the rapid advancement of high‐power, miniaturized electronic devices, the demand for high‐efficiency thermal management materials has grown increasingly urgent. In this work, a macromolecular silicone crosslinker (VPS) with dynamic imine bonds was synthesized via a Schiff base reaction and subsequently used to cure and crosslink epoxy monomers. By adjusting the crosslinker content, a flexible epoxy resin matrix containing dynamic covalent bonds (EVPS) was fabricated. Furthermore, the thermal conductivity of the epoxy resin was enhanced by incorporating boron nitride (BN) fillers. The results indicated that when the addition ratio of BN reached 50%, the thermal conductivity of the composite significantly increased to 3.34 W m −1 K −1 . The potential of such composites as thermal management materials was verified in a practical heat‐dissipation scenario for LED chips. Notably, the composites prepared in this study could be degraded under chemical conditions, after which the fillers could be separated via physical filtration. This method is expected to provide a novel, efficient, and environmentally friendly solution for the sustainable development of thermal management materials.