Multistage self-assembly strategy: Designed synthesis of n-doped mesoporous carbon with high and controllable pyridine N content for ultrahigh surface-area-normalized capacitance

Nitrogen doping could improve the performance of carbon materials in electrocatalysis, CO₂ adsorption, and energy storage. ^[1]However, the control of the doping type and the amount of nitrogen (N)-doped in carbon materials in a simple and environmentally friendly way remains challenging. Herein, we report a facile, multistage, self-assembly strategy for the synthesis of two-dimensional N-doped mesoporous carbon (2D NMC) by using graphene oxide (GO) as a structure-directing agent. The resultant 2D GO@NMCs rendered quantitatively controllable mesopores (8–25 nm). The 2D GO@NMCs rendered quantitatively controllable mesopores (8–25 nm), high and controllable N content (up to 19 wt %), and the percentages of pyridine and pyridone/pyrrolic N atoms were as high as 49.9% and 35.3%, respectively. Due to these unique characteristics, the fabricated 2D GO@NMCs exhibited an ultrahigh surface-area-normalized capacitance of up to 90.6 μF cm⁻², which was much higher than the theoretical electrochemical double-layer capacitance of activated carbon (15–25 μF cm⁻²). Moreover, our proposed multistage self-assembly strategy is versatile, and thus, could be extended to the synthesis of one-dimensional (1D) nanotubes@NMC and zero-dimensional (0D) nanospheres@NMC materials.