Assembly Multifunctional Three-Dimensional Carbon Networks by Controlling Intermolecular Forces

Three-dimensional (3D) carbon networks (3DCNs) enjoy the merits of high surface area, effective mass-transfer ability, and mechanical stability. The physicochemical properties of such materials not only depend on their microstructures but also rely on the assembly forms. This work achieves different assembly forms of 3DCNs on the macroscale from powder, monolith, to clay and reveals the relations between intermolecular forces and these assembly forms. With the “weak” van der Waals forces, only 3DCN powders are obtained. The N-doping effect increases the part of “strong” van der Waals forces, which enables 3DCNs assembled as a monolith and supports 43 000 times its own weight. Furthermore, the introduction of aniline molecules and the corresponding hydrogen bond connections make carbon networks to transform into a clay with superior ductility and plasticity. Considering that 3DCNs can be engineered into functionalized materials by in situ incorporation of functional components such as Fe₃O₄, the composites with controllable forms are treated as promising candidate materials used in various fields.