Rational Design of Carbon-Based Porous Aerogels with Nitrogen Defects and Dedicated Interfacial Structures toward Highly Efficient CO(2) Greenhouse Gas Capture and Separation

[Image: see text] CO(2) capture from flowing flue gases through adsorption technology is essential to reduce the emission of CO(2) 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 ZnCl(2) 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 CO(2) capture and further improve the CO(2)/N(2) separation efficiencies. Among the prepared samples, NCA-1-2 with a high micropore surface area and high nitrogen content exhibits a high CO(2) adsorption capacity (4.30 mmol g(–1) at 0 °C and 1 bar) and CO(2)/N(2) 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 CO(2) adsorption capacity, high selectivity, and adsorption performance remained pretty stable after multiple uses.