Graphene/Graphitized Polydopamine/Carbon Nanotube All-Carbon Ternary Composite Films with Improved Mechanical Properties and Through-Plane Thermal Conductivity

Graphene films (GFs) are promising ultrathin thermally conductive materials for portable electronic devices because of their excellent thermally conductive property, light weight, high flexibility, and low cost. However, the application of GFs is limited due to their poor mechanical properties and through-plane thermal conductivity. Here, a graphene-(graphitized polydopamine)-(carbon nanotube) (G-gPDA-CNT) all-carbon ternary composite film was fabricated by chemical reduction, carbonization, graphitization, and mechanical compaction of the evaporation-assembled (graphene oxide)-PDA@CNT film. The G-gPDA-CNT film exhibited a uniform all-carbon composite structure in which the components of the graphene, gPDA layers, and CNTs were cross-linked by strong covalent bonds. This unique structure promoted the load transfer and energy dissipation between the components by which the mechanical properties of the G-gPDA-CNT film were substantially improved. Furthermore, electron and phonon transfers were also promoted, greatly improving the electrical and thermal conductivities, especially the through-plane thermal conductivity of the G-gPDA-CNT film. The G-gPDA-CNT film showed a tensile strength of 67.5 MPa, 15.1% ultimate tensile strain, toughness of 6.07 MJ/m3, electrical conductivity of 6.7 × 105 S·m–1, in-plane thermal conductivity of 1597 W·m–1·K–1, and through-plane thermal conductivity of 2.65 W·m–1·K–1, which were 2.24, 1.44, 3.16, 1.46, 1.15, and 3.90 times that of the pure GFs, respectively.