Effects of Sulfur Doping and Humidity on CO2 Capture by Graphite Split Pore: A Theoretical Study.

By use of grand canonical Monte Carlo calculations, we study the effects of sulfur doping and humidity on the performance of graphite split pore as an adsorbent for CO2 capture. It is demonstrated that S doping can greatly enhance pure CO2 uptake by graphite split pore. For example, S-graphite split pore with 33.12% sulfur shows a 39.85% rise in pure CO2 uptake (51.001 mmol/mol) compared with pristine graphite split pore at 300 K and 1 bar. More importantly, it is found that S-graphite split pore can still maintain much higher CO2 uptake than that by pristine graphite split pore in the presence of water. Especially, uptake by 33.12% sulfur-doped S-graphite split pore is 51.963 mmol of CO2/mol in the presence of water, which is 44.34% higher than that by pristine graphite split pore at 300 K and 1 bar. In addition, CO2/N2 selectivity of S-graphite split pore increases with increasing S content, resulting from stronger interactions between CO2 and S-graphite split pore. Moreover, by use of density functional theory calculations, we demonstrate that S doping can enhance adsorption energy between CO2 molecules and S-graphene surface at different humidities and furthermore enhance CO2 uptake by S-graphite split pore. Our results indicate that S-graphite split pore is a promising adsorbent material for humid CO2 capture.