Covalent bond-assisted continuous interface structure for high thermal conductive polyimide composite films

Polyimide (PI) is widely used in electronic, electrical and communication fields because of its outstanding mechanical properties, electrical insulation and thermal stability. However, the lower thermal conductivity limits their application. Here, PI composite films with high thermal conductivity are obtained by utilizing reactive groups on the carbon nitride nanosheets (CNNS) surface to form covalent bond with PI matrix. The thermal conductivity of CNNS/PI composite films can reach 5.84 W∙m⁻¹∙K⁻¹, which is about 10 times higher than that of pure PI (0.56 W∙m⁻¹∙K⁻¹). This is attributed to the covalent bond between CNNS and PI matrix acting as a “thermal bridge” to connect the discontinuities at the interface, thereby reducing the interfacial thermal resistance between CNNS and PI. The heat transfer mechanism of composite film is further revealed by finite element analysis. This work provides a viable solution to improve the thermal conductivity of PI, allowing for a wide range of potential applications for PI in electronic devices.