Chemical Foaming Coupled Self-Etching: A Multiscale Processing Strategy for Ultrahigh-Surface-Area Carbon Aerogels

Due to the unique structure, carbon aerogels have always shown great potential for multifunctional applications. At present, it is highly desirable but remains challenging to tailor the microstructures with respect to porosity and specific surface area to further expand its significance. A facile chemical foaming coupled self-etching strategy is developed for multiscale processing of carbon aerogels. The strategy is directly realized via the pyrolysis of a multifunctional precursor (pentaerythritol melamine phosphate) without any special drying process and multiple steps. In the micrometer scale, the macroporous scaffold structures with interconnected and strutted carbon nanosheets are built up by chemical foaming from decomposition of melamine, whereas the meso/microporous nanosheets are formed via self-etching by phosphorus-containing species. The delicately hierarchical structures and record-breaking specific surface area of 2668.4 m² g^–1 render the obtained carbon aerogels great potentials for absorption (324.1–593.6 g g^–1 of absorption capacities for varied organic solvents) and energy storage (338 F g^–1 of specific capacitance). The construction of such novel carbon nanoarchitecture will also shed light on the design and synthesis of multifunctional materials.