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Reduced graphene oxide (rGO) aerogels with a three-dimensional (3D) interconnected network provides continuous heat transport paths in multi-directions. However, the high porosity of rGO aerogels commonly leads to very low thermal conductivity (TC), and defects and grain boundaries of rGO sheets result in a high extent of phonon scattering, which is far from satisfying the requirement of thermal interface materials (TIMs). Here, a compressible graphitized-rGO/polyimide (g-rGO/PI) aerogel was prepared by the ice-template method and "molecular welding" strategy. The regular cellular structure and closely packed cell walls bring the g-rGO/PI aerogel high compressibility, which made the aerogel can maintain the continuous thermal transport paths well even in highly compacted status. The rGO sheets in the cell wall surface are welded up by g-PI during imidization and graphitization treatment, providing efficient channels for phonon transportation in the 3D network. The g-rGO/PI aerogel in a compressive strain of 95% has a high TC in the plane of 172.5 W m -1 k -1 and a high TC through the plane of 58.1 W m -1 k -1 , which is superior to other carbon-based TIMs previously reported.

Graphitized-rGO/Polyimide Aerogel as the Compressible Thermal Interface Material with Both High in-Plane and through-Plane Thermal Conductivities