Flyweight 3D Graphene Scaffolds with Microinterface Barrier-Derived Tunable Thermal Insulation and Flame Retardancy

In this article, flyweight three-dimensional (3D) graphene scaffolds (GSs) have been demonstrated with a microinterface barrier-derived thermal insulation and flame retardancy characteristics. Such 3D GSs were fabricated by a modified hydrothermal method and a unidirectional freeze-casting process with hierarchical porous microstructures. Because of high porosity (99.9%), significant phonon scattering, and strong π-π interaction at the interface barriers of multilayer graphene cellular walls, the GSs demonstrate a sequence of multifunctional properties simultaneously, such as lightweight density, thermal insulating characteristics, and outstanding mechanical robustness. At 100 °C, oxidized GSs exhibit a thermal conductivity of 0.0126 ± 0.0010 W/(m K) in vacuum. The thermal conductivity of oxidized GSs remains relatively unaffected despite large-scale deformation-induced densification of the microstructures, as compared to the behavior of reduced GSs (rGSs) whose thermal conductivity increases dramatically under compression. The contrasting behavior of oxidized GSs and rGSs appears to derive from large differences in the intersheet contact resistance and varying intrinsic thermal conductivity between reduced and oxidized graphene sheets. The oxidized GSs also exhibit excellent flame retardant behavior and mechanical robustness, with only 2% strength decay after flame treatment. In a broader context, this work demonstrates a useful strategy to design porous nanomaterials with a tunable heat conduction behavior through interface engineering at the nanoscale.