Recyclable and elastic highly thermally conductive epoxy-based composites with covalent-noncovalent interpenetrating networks.

High-power electronic architectures and devices require elastic thermally conductive materials. The use of epoxy resin in thermal management is limited due to its rigidity. Here, based on epoxy vitrimer, flexible polyethylene glycol (PEG) chains are introduced into covalent adaptable networks to construct covalent-noncovalent interpenetrating networks, enabling the elasticity of epoxy resins. Compared to traditional silicone-based thermal interface materials, the newly developed elastic epoxy resin shows the advantages of reprocessability, self-healing, and no small molecule release. Results show that, even after being filled with boron nitride and liquid metal, the material maintains its resilience, reprocessability and self-healing properties. Leveraging these characteristics, the composite can be further processed into thin films through a repeated pressing-rolling technique that facilitates the forced orientation of the fillers. Subsequently, the bulk composites are reconstructed using a film-stacking method. The results indicate that the thermal conductivity of the reconstructed bulk composite reaches 3.66 W m-1 K-1, achieving a 68% increase compared to the composite prepared through blending. Due to the existence of covalent adaptable networks, the inorganic and inorganic components of the composite prepared in this work can be completely separated under mild conditions, realizing closed-loop recycling.