Development of high-performance materials
for the capture
and separation
of CO2 from the gas mixture is significant to alleviate
carbon emission and mitigate the greenhouse effect. In this work,
a novel structure of C9N7 slit was developed
to explore its CO2 adsorption capacity and selectivity
using Grand Canonical Monte Carlo (GCMC) and Density Functional Theory
(DFT) calculations. Among varying slit widths, C9N7 with the slit width of 0.7 nm exhibited remarkable CO2 uptake with superior CO2/N2 and CO2/CH4 selectivity. At 1 bar and 298 K, a maximum
CO2 adsorption capacity can be obtained as high as 7.06
mmol/g, and the selectivity of CO2/N2 and CO2/CH4 was 41.43 and 18.67, respectively. In the
presence of H2O, the CO2 uptake of C9N7 slit decreased slightly as the water content increased,
showing better water tolerance. Furthermore, the underlying mechanism
of highly selective CO2 adsorption and separation on the
C9N7 surface was revealed. The closer the adsorption
distance, the stronger the interaction energy between the gas molecule
and the C9N7 surface. The strong interaction
between the C9N7 nanosheet and the CO2 molecule contributes to its impressive CO2 uptake and
selectivity performance, suggesting that the C9N7 slit could be a promising candidate for CO2 capture and
separation.