Highly nitrogen-enriched mesoporous carbon nitride materials with 2-dimensional (2-D) (2D-meso-CN) and 3-dimensional (3-D) mesostructures (3D-meso-CN) were synthesized using mesoporous silica as a hard template and cyanamide as a precursor via the incipient wetness process without using any solvent. The materials were characterized by small-angle X-ray scattering (SAXS), X-ray diffraction (XRD), and transmission electron microscopy (TEM) for the mesostructure analysis, N₂ adsorption–desorption isotherms for surface area and pore size distribution, and X-ray photoelectron spectroscopy (XPS) and Fourier-transform infrared (FT-IR) spectroscopy for the composition analysis of frameworks. The mesoporous carbon nitride replicas have graphitic-like stacking of carbon nitride sheets in mesopore walls. The N/C ratio of the mesoporous carbon nitride replicas is 1.13 after the carbonization at 550 °C for 3 h. 2D-meso-CN and 3D-meso-CN have the BET surface area of 361 and 343 m² g⁻¹, large pore volume of 0.50 and 0.67 cm³ g⁻¹, and pore diameter of 27.8 Å (for 2D-meso-CN), 24.5 and 80.3 Å (for 3D-meso-CN), respectively. It was found that the 3D-meso-CN has higher capacity of hydrogen uptake of 0.25 wt% than the pure mesoporous carbon FDU-15 (0.16 wt%) at 50 bar under room temperature (298 K).

A simple strategy for the synthesis of macro-mesoporous carbonaceous monolith materials has been demonstrated through an organic-organic self-assembly at the interface of an organic scaffold such as polyurethane (PU) foam. Hierarchically porous carbonaceous monoliths with cubic (Im \( \bar 3 \) m) or hexagonal (p6mm) mesostructure were prepared through evaporation induced self-assembly of the mesostructure on the three-dimensional (3-D) interconnecting struts of the PU foam scaffold. The preparation was carried out by using phenol/formaldehyde resol as a carbon precursor, triblock copolymer F127 as a template for the mesostructure and PU foam as a sacrificial monolithic scaffold. Their hierarchical pore system was macroscopically fabricated with cable-like mesostructured carbonaceous struts. The carbonaceous monoliths exhibit macropores of diameter 100–450 μm, adjustable uniform mesopores (3.8–7.5 nm), high surface areas (200–870 m²/g), and large pore volumes (0.17–0.58) cm³/g. Compared with the corresponding evaporation induced self-assembly (EISA) process on a planar substrate, this facile process is a time-saving, labor-saving, space-saving, and highly efficient pathway for mass production of ordered mesoporous materials.