Thermally conductive, self-healing, and elastic Polyimide@Vertically aligned carbon nanotubes composite as smart thermal interface material

Smart thermal interface materials must exhibit self-healability and high thermal conductivity (k) and elastic deformation as they can experience repeated compression and undergo sudden damage. However, it remains challenging to ensure high phonon mobility/efficient phonon transfer, self-healing, and good elasticity by optimizing its molecular orientation or cross-links. Herein, a self-healing and elastic polyimide copolymer (EMPI) cross-linked by flexible and rigid segments is uniformly filled into the gaps of a forest of vertically aligned carbon nanotubes (VACNTs). The [email protected] composite exhibits a high k value at 10.83 ± 0.22 W m−1 K−1, low interfacial thermal resistance at 6.83 ± 0.15 K mm2 W−1, high elastic compressive deformation (30% at 2.5 MPa), and strong surface adhesion (0.3 MPa). Further, it could recover 90.8% of its elastic modulus and 92% of its thermal resistance after self-healing at 80 °C for 80 h. An [email protected] device exhibits efficient heat conduction not only by recovering after gradient compressive strains of up to 30% but also by self-healing its damage or reforming the interface with Cu. Thus, the thermally conductive, self-healing, and elastic [email protected] composite opens new avenues for smart thermal management in various high-power/intelligent devices.