Carbon Dioxide Capture by Adsorption in a Model Hydroxy-Modified Graphene Pore

Concerns regarding the environmental impact of increasing levels of anthropogenic carbon dioxide have led to a variety of studies examining solid surfaces for their ability to trap this greenhouse gas (GHG). Atmospheric or post-combustion carbon capture requires an efficient separation of carbon dioxide and nitrogen gas. We used the molecular mechanics MM3 parameter set (previously shown to provide good estimates of molecule–surface binding energies) to calculate theoretical surface binding energies for carbon dioxide ∆E(CO(2)) and nitrogen ∆E(N(2)). For efficient separation, differentiation of these two gas-surface adsorption energies is required. Examined structures based on graphene, carbon slit width pore, and carbon nanotube gave ∆E(CO(2)) to ∆E(N(2)) ratios of 1.7, 1.8, and 1.9, respectively. To enhance the CO(2) adsorption, we developed a model graphene surface pore lined with four hydroxy groups whose orientation allowed them to form hydrogen bonds with the oxygens in CO(2). Both the single-layer and double-layer versions of this pore gave significant enhancement in the ability to trap CO(2) preferentially to N(2). The two-layer version of this pore gave ∆E(CO(2)) = 73 and ∆E(N(2)) = 6.8 kJ/mol. The one- and two-layer versions of this novel pore averaged a ∆E(CO(2)) to ∆E(N(2)) ratio of 12.