Abstract
The transport of water through nanoscale capillaries/pores plays a prominent role in biology, ionic/molecular separations, water treatment and protective applications. However, the mechanisms of water and vapor transport through nanoscale confinements remain to be fully understood. Angstrom-scale pores (~2.8–6.6 Å) introduced into the atomically thin graphene lattice represent ideal model systems to probe water transport at the molecular-length scale with short pores (aspect ratio ~1–1.9) i.e., pore diameters approach the pore length (~3.4 Å) at the theoretical limit of material thickness. Here, we report on orders of magnitude differences (~80×) between transport of water vapor (~44.2–52.4 g m−2 day−1 Pa−1) and liquid water (0.6–2 g m−2 day−1 Pa−1) through nanopores (~2.8–6.6 Å in diameter) in monolayer graphene and rationalize this difference via a flow resistance model in which liquid water permeation occurs near the continuum regime whereas water vapor transport occurs in the free molecular flow regime. We demonstrate centimeter-scale atomically thin graphene membranes with up to an order of magnitude higher water vapor transport rate (~5.4–6.1 × 104g m−2 day−1) than most commercially available ultra-breathable protective materials while effectively blocking even sub-nanometer (>0.66 nm) model ions/molecules.
| Original language | English |
|---|---|
| Article number | 6709 |
| Journal | Nature Communications |
| Volume | 13 |
| Issue number | 1 |
| DOIs | |
| State | Published - Dec 2022 |
Funding
The use of Vanderbilt Institute of Nanoscale Science and Engineering CORE facilities and Prof. Carlos Silvera Batista’s Lab for UV/ozone etching are acknowledged. This work was supported in part by NSF CAREER award #1944134, ACS PRF Grant number 59267-DNI10, and faculty start-up funds to P.R.K. from Vanderbilt University. The STEM and STM experiments were conducted at the Center for Nanophase Materials Sciences at Oak Ridge National Laboratory, which is a DOE Office of Science User Facility. Molecular dynamics simulations were performed in LAMMPS90(http://lammps.sandia.gov) and visualized in VMD (visual molecular dynamics)91. This work made use of computing resources of the Shared Hierarchical Academic Research Computing Network (SHARCNET: www.sharcnet.ca) and Compute Canada (www.computecanada.ca). F.F. and M.L.J. acknowledge financial support from the Chemical and Biological Technologies Department of the Defense Threat Reduction Agency (DTRA-CB) via grant BA12PHM123 in the “Dynamic Multifunctional Materials for a Second Skin D[MS]2” program. Work at LLNL was performed under the auspices of the US Department of Energy under contract DEAC52-07NA27344. The use of Vanderbilt Institute of Nanoscale Science and Engineering CORE facilities and Prof. Carlos Silvera Batista’s Lab for UV/ozone etching are acknowledged. This work was supported in part by NSF CAREER award #1944134, ACS PRF Grant number 59267-DNI10, and faculty start-up funds to P.R.K. from Vanderbilt University. The STEM and STM experiments were conducted at the Center for Nanophase Materials Sciences at Oak Ridge National Laboratory, which is a DOE Office of Science User Facility. Molecular dynamics simulations were performed in LAMMPS ( http://lammps.sandia.gov ) and visualized in VMD (visual molecular dynamics). This work made use of computing resources of the Shared Hierarchical Academic Research Computing Network (SHARCNET: www.sharcnet.ca ) and Compute Canada ( www.computecanada.ca ). F.F. and M.L.J. acknowledge financial support from the Chemical and Biological Technologies Department of the Defense Threat Reduction Agency (DTRA-CB) via grant BA12PHM123 in the “Dynamic Multifunctional Materials for a Second Skin D[MS]” program. Work at LLNL was performed under the auspices of the US Department of Energy under contract DEAC52-07NA27344. 2
