Department of Chemical and Biomolecular Engineering, Vanderbilt University, Nashville, TN, 37212, USA.
Physical and Life Sciences, Lawrence Livermore National Laboratory, Livermore, CA, 94550, USA.
Nat Commun. 2022 Nov 7;13(1):6709. doi: 10.1038/s41467-022-34172-1.
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 day Pa) and liquid water (0.6-2 g m day Pa) 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 × 10g m day) than most commercially available ultra-breathable protective materials while effectively blocking even sub-nanometer (>0.66 nm) model ions/molecules.
水在纳米级毛细管/孔隙中的传输在生物学、离子/分子分离、水处理和防护应用中起着重要作用。然而,水和蒸汽通过纳米级封闭空间的传输机制仍有待充分理解。在原子级薄的石墨烯晶格中引入的埃级孔隙(2.8-6.6 Å)代表了理想的模型系统,可以在分子长度尺度上探测水的传输,短孔隙(纵横比1-1.9),即孔径接近理论上材料厚度的极限(3.4 Å)。在这里,我们报告了水蒸气(44.2-52.4 g m day Pa)和液态水(0.6-2 g m day Pa)通过单层石墨烯中的纳米孔(直径2.8-6.6 Å)的传输存在数量级差异(80×),并通过流阻模型对此差异进行了合理化解释,该模型认为液态水的渗透发生在连续区附近,而水蒸气的传输发生在自由分子流区。我们展示了厘米级原子薄的石墨烯膜,其水蒸气传输速率比大多数市售的超透气防护材料高一个数量级(~5.4-6.1×10g m day),同时有效阻止了甚至亚纳米级(>0.66 nm)的模型离子/分子。