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.