Porous carbon nanosheets with precisely tunable thickness and selective CO2 adsorption properties

Abstract

We report the wet-chemistry synthesis of a new type of porous carbon nanosheet whose thickness can be precisely controlled over the nanometer length scale. This feature is distinct from conventional porous carbons that are composed of micron-sized or larger skeletons, and whose structure is less controlled. The synthesis uses graphene oxide (GO) as the shape-directing agent and asparagine as the bridging molecule that connects the GO and in situ grown polymers by electrostatic interaction between the molecules. The assembly of the nanosheets can produce macroscopic structures, i.e., hierarchically porous carbon monoliths which have a mechanical strength of up to 28.9 MPa, the highest reported for the analogues. The synthesis provides precise control of porous carbons over both microscopic and macroscopic structures at the same time. In all syntheses the graphene content used was in the range 0.5–2.6 wt%, which is significantly lower than that of common surfactants used in the synthesis of porous materials. This indicates the strong shape-directing function of GO. In addition, the overall thickness of the nanosheets can be tuned from 20 to 200 nm according to a fitted linear correlation between the carbon precursor/GO mass ratio and the coating thickness. The porous carbon nanosheets show impressive CO₂ adsorption capacity under equilibrium, good separation ability of CO₂ from N₂ under dynamic conditions, and easy regeneration. The highest CO₂ adsorption capacities can reach 5.67 and 3.54 CO₂ molecules per nm³ pore volume and per nm² surface area at 25 °C and ∼1 bar.