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Much attention has been paid to graphite flakes/copper (GFs/Cu) composites for thermal management due to their remarkable thermal properties. Most studies focus on the interface interaction between GFs and Cu in composites. However, controlling the orientation of GFs still remains a challenge. Herein, we report a reliable method to ensure consistent orientation of GFs in the composites. Firstly, the disorder GFs were well arranged on the surface of copper foil by tape casting process in the casting machine. Then highly aligned GFs/Cu composites were fabricated by hot pressing process in a vacuum hot-pressing furnace, with the volume fraction of graphite from 30% to 70%. The SEM images show that the obtained GFs/Cu composites presented a layer-by-layer structure or network structure with a different content of GFs. The thermal conductivity of GFs/Cu composites exhibited an extreme anisotropy due to the highly aligned GFs. The ultrahigh thermal conductivity of GFs/Cu composites with 70 vol% GFs reached 741 W/(m·K), while through-plane thermal conductivity was just 42 W/(m·K). The alignment of GFs and interfacial thermal resistance were deeply analyzed and a thermal conductivity model for GFs/Cu composites was established. Our work provides a new idea to significantly enhance the thermal transportation performance of GFs/Cu composites by well controlled alignment of GFs in Cu matrix.

High Thermal Conductivity and Anisotropy Values of Aligned Graphite Flakes/Copper Foil Composites