Three-dimensional carbon nanonetworks (3D CNNs) have become a research hotspot of high-performance electrode materials due to their unique conductive framework and connected porous structure. Among them, the 3D CNNs prepared from high aspect ratio nanometers retained the mass transfer advantage of two-dimensional building elements, which was conducive to the further improvement of its electrochemical performance. However, conventional 3D CNNs are usually formed by physical lapping of network units, which lack chemical covalent bonds, and are difficult to form stable long-range 3D structures. In addition, the lapping and stacking of construction units mainly form large-size mesopores and macropores, while the micropores and small-size mesopores providing the active site are relatively scarce. Although micropores or small mesos can be introduced by post-processing or additional template, the process is cumbersome and the structure controllability is poor. Therefore, there are still great challenges in the development of simple and efficient preparation of high-performance 3D CNNs.

A new strategy is based on a two-dimensional molecular brush of GO grafted with polyacrylaldehyde (GO-G-PA) as the building unit, and tetral (4-aminophenyl) methane (TAPM) as the cross-linking agent. A kind of superlayered carbon sheet network (SHCNN) with nitrogen doped carbon layer, micro - medium - Dalian channel and long-range conductive framework was constructed by simple Schiff base reaction and subsequent carbonization process.