Abstract
Pore size is a crucial factor impacting gas separation in porous separation materials, but how to control the pore size to optimize the separation performance remains a challenge. Here, we propose a design of graphene/ionic liquid composites with tunable slit pore sizes, where cations and anions of ionic liquids are intercalated between graphene layers. By varying the sizes of the ions, we show from first-principles density functional theory calculations that the accessible pore size can be tuned from 3.4 to 6.0 Å. Grand canonical Monte Carlo simulations of gas sorption find that the composite materials possess high CO2 uptake at room temperature and 1 bar (up to ∼8.5 mmol/g). Further simulations of the sorption of gas mixtures reveal that high CO2/N2 and CO2/CH4 adsorption selectivities can be obtained when the accessible pore size is <5 Å. This work suggests a new strategy to achieve tunable pore sizes via the graphene/IL composites for highly selective CO2/N2 and CO2/CH4 adsorption.
| Original language | English |
|---|---|
| Pages (from-to) | 17511-17516 |
| Number of pages | 6 |
| Journal | ACS Applied Materials and Interfaces |
| Volume | 13 |
| Issue number | 15 |
| DOIs | |
| State | Published - Apr 21 2021 |
Funding
This work was sponsored by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231.
| Funders | Funder number |
|---|---|
| U.S. Department of Energy | |
| Office of Science | DE-AC02-05CH11231 |
| Basic Energy Sciences | |
| Chemical Sciences, Geosciences, and Biosciences Division |
Keywords
- density functional theory
- gas separation
- grand canonical Monte Carlo
- graphene
- ionic liquid
- pore size
