Rational Design of Carbon-Based Porous Aerogels with Nitrogen Defects and Dedicated Interfacial Structures toward Highly Efficient CO2 Greenhouse Gas Capture and Separation

CO2 capture from flowing flue gases through adsorption technology is essential to reduce the emission of CO2 to the atmosphere. The rational design of highly efficient carbon-based absorbents with interfacial structures containing interconnected porous structures and abundant adsorption sites might be one of the promising strategies. Here, we report the synthesis of nitrogen-doped carbon aerogels (NCAs) via prepolymerized phenol–melamine–formaldehyde organic aerogels (PMF) by controlling the addition amount of ZnCl2 and the precursor M/P ratio. It has been revealed that NCAs with a higher specific surface area and interconnected porous structures contain a large amount of pyridinic nitrogen and pyrrolic nitrogen. These would act as the intrinsic adsorption sites for highly effective CO2 capture and further improve the CO2/N2 separation efficiencies. Among the prepared samples, NCA-1-2 with a high micropore surface area and high nitrogen content exhibits a high CO2 adsorption capacity (4.30 mmol g–1 at 0 °C and 1 bar) and CO2/N2 selectivity (36.5 at 25 °C, IAST). Under typical flue gas conditions (25 °C and 1.01 bar), equilibrium gas adsorption analysis and dynamic breakthrough measurement associated with a high adsorption capacity of 2.65 mmol g–1 at 25 °C and 1.01 bar and 0.81 mmol g–1 at 25 °C and 0.15 bar. This rationally designed N-doped carbon aerogel with specific interfacial structures and high CO2 adsorption capacity, high selectivity, and adsorption performance remained pretty stable after multiple uses.