By creating nanoscale pores in a layer of graphene, it could be used as an effective separation membrane due to its chemical and mechanical stability, its flexibility and, most importantly, its one-atom thickness. Theoretical studies have indicated that the performance of such membranes should be superior to state-of-the-art polymer-based filtration membranes, and experimental studies have recently begun to explore their potential. Here, we show that single-layer porous graphene can be used as a desalination membrane. Nanometre-sized pores are created in a graphene monolayer using an oxygen plasma etching process, which allows the size of the pores to be tuned. The resulting membranes exhibit a salt rejection rate of nearly 100% and rapid water transport. In particular, water fluxes of up to 106 g m−2 s−1 at 40 °C were measured using pressure difference as a driving force, while water fluxes measured using osmotic pressure as a driving force did not exceed 70 g m−2 s−1 atm−1.
Subscribe to Journal
Get full journal access for 1 year
only $14.08 per issue
All prices are NET prices.
VAT will be added later in the checkout.
Rent or Buy article
Get time limited or full article access on ReadCube.
All prices are NET prices.
Shannon, M. A. et al. Science and technology for water purification in the coming decades. Nature 452, 301–310 (2008).
Elimelech, M. & Phillip, W. A. The future of seawater desalination: energy, technology, and the environment. Science 333, 712–717 (2011).
Cohen-Tanugi, D., McGovern, R. K., Dave, S. H., Lienhard, J. H. & Grossman, J. C. Quantifying the potential of ultra-permeable membranes for water desalination. Energy Environ. Sci. 7, 1134–1141 (2014).
Nair, R. R., Wu, H. A., Jayaram, P. N., Grigorieva, I. V. & Geim, A. K. Unimpeded permeation of water through helium-leak-tight graphene-based membranes. Science 335, 442–444 (2012).
Cohen-Tanugi, D. & Grossman, J. C. Water desalination across nanoporous graphene. Nano Lett. 12, 3602–3608 (2012).
Jiang, D-E., Cooper, V. R. & Dai, S. Porous graphene as the ultimate membrane for gas separation. Nano Lett. 9, 4019–4024 (2009).
Konatham, D., Yu, J., Ho, T. A. & Striolo, A. Simulation insights for graphene-based water desalination membranes. Langmuir 29, 11884–11897 (2013).
Suk, M. E. & Aluru, N. R. Water transport through ultrathin graphene. J. Phys. Chem. Lett. 1, 1590–1594 (2010).
Du, H. et al. Separation of hydrogen and nitrogen gases with porous graphene membrane. J. Phys. Chem. C 115, 23261–23266 (2011).
Sint, K., Wang, B. & Kral, P. Selective ion passage through functionalized graphene nanopores. J. Am. Chem. Soc. 130, 16448–16449 (2008).
Sun, C. et al. Mechanisms of molecular permeation through nanoporous graphene membranes. Langmuir 30, 675–682 (2014).
Wang, E. N. & Karnik, R. Water desalination graphene cleans up water. Nature Nanotech. 7, 552–554 (2012).
Koenig, S. P., Wang, L., Pellegrino, J. & Bunch, J. S. Selective molecular sieving through porous graphene. Nature Nanotech. 7, 728–732 (2012).
Kim, H. W. et al. Selective gas transport through few-layered graphene and graphene oxide membranes. Science 342, 91–95 (2013).
Li, H. et al. Ultrathin, molecular-sieving graphene oxide membranes for selective hydrogen separation. Science 342, 95–98 (2013).
Garaj, S. et al. Graphene as a subnanometre trans-electrode membrane. Nature 467, 190–193 (2010).
Shan, Y. P. et al. Surface modification of graphene nanopores for protein translocation. Nanotechnology 24, 495102 (2013).
O'Hern, S. C. et al. Selective ionic transport through tunable subnanometer pores in single-layer graphene membranes. Nano Lett. 14, 1234–1241 (2014).
O'Hern, S. C. et al. Selective molecular transport through intrinsic defects in a single layer of CVD graphene. ACS Nano 6, 10130–10138 (2012).
Vlassiouk, I. et al. Large scale atmospheric pressure chemical vapor deposition of graphene. Carbon 54, 58–67 (2013).
Vlassiouk, I., Apel, P. Y., Dmitriev, S. N., Healy, K. & Siwy, Z. S. Versatile ultrathin nanoporous silicon nitride membranes. Proc. Natl Acad. Sci. USA 106, 21039–21044 (2009).
Malard, L. M., Pimenta, M. A., Dresselhaus, G. & Dresselhaus, M. S. Raman spectroscopy in graphene. Phys. Rep. 473, 51–87 (2009).
Vlassiouk, I. et al. Graphene nucleation density on copper: fundamental role of background pressure. J. Phys. Chem. C 117, 18919–18926 (2013).
Dresselhaus, M. S., Jorio, A., Hofmann, M., Dresselhaus, G. & Saito, R. Perspectives on carbon nanotubes and graphene Raman spectroscopy. Nano Lett. 10, 751–758 (2010).
Lucchese, M. M. et al. Quantifying ion-induced defects and Raman relaxation length in graphene. Carbon 48, 1592–1597 (2010).
Bunch, J. S. et al. Impermeable atomic membranes from graphene sheets. Nano Lett. 8, 2458–2462 (2008).
Smirnov, S. N., Vlassiouk, I. V. & Lavrik, N. V. Voltage-gated hydrophobic nanopores. ACS Nano 5, 7453–7461 (2011).
Cohen-Tanugi, D. & Grossman, J. C. Water permeability of nanoporous graphene at realistic pressures for reverse osmosis desalination. J. Chem. Phys. 141, 074704 (2014).
Goosen, M. F. A. et al. Fouling of reverse osmosis and ultrafiltration membranes: a critical review. Sep. Sci. Technol. 39, 2261–2297 (2004).
Guo, J. et al. Crown ethers in graphene. Nature Commun. 5, 5389 (2014).
Lee, J. et al. Stabilization of graphene nanopore. Proc. Natl Acad. Sci. USA 111, 7522–7526 (2014).
Surwade, S. P., Li, Z. T. & Liu, H. T. Thermal oxidation and unwrinkling of chemical vapor deposition-grown graphene. J. Phys. Chem. C 116, 20600–20606 (2012).
Liu, L. et al. Graphene oxidation: thickness-dependent etching and strong chemical doping. Nano Lett. 8, 1965–1970 (2008).
Diankov, G., Neumann, M. & Goldhaber-Gordon, D. Extreme mono layer-selectivity of hydrogen-plasma reactions with graphene. ACS Nano 7, 1324–1332 (2013).
Banhart, F., Kotakoski, J. & Krasheninnikov, A. V. Structural defects in graphene. ACS Nano 5, 26–41 (2011).
Wang, B., Puzyrev, Y. & Pantelides, S. T. Strain enhanced defect reactivity at grain boundaries in polycrystalline graphene. Carbon 49, 3983–3988 (2011).
Majumder, M., Chopra, N., Andrews, R. & Hinds, B. J. Nanoscale hydrodynamics—enhanced flow in carbon nanotubes. Nature 438, 44–44 (2005).
Holt, J. K. et al. Fast mass transport through sub-2-nanometer carbon nanotubes. Science 312, 1034–1037 (2006).
Severin, N., Lange, P., Sokolov, I. M. & Rabe, J. P. Reversible dewetting of a molecularly thin fluid water film in a soft graphene-mica slit pore. Nano Lett. 12, 774–779 (2012).
Datta, D., Li, J. W. & Shenoy, V. B. Defective graphene as a high-capacity anode material for Na- and Ca-ion batteries. ACS Appl. Mater. Interfaces 6, 1788–1795 (2014).
Research sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the US Department of Energy. Research also supported through a user proposal at ORNL's Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility.
The authors declare no competing financial interests.
About this article
Cite this article
Surwade, S., Smirnov, S., Vlassiouk, I. et al. Water desalination using nanoporous single-layer graphene. Nature Nanotech 10, 459–464 (2015). https://doi.org/10.1038/nnano.2015.37
Controlled defect formation and heteroatom doping in monolayer graphene using active oxygen species under ultraviolet irradiation
Chemical Society Reviews (2020)
Materials Today Communications (2020)
The effect of chemical functional groups and salt concentration on performance of single-layer graphene membrane in water desalination process: A molecular dynamics simulation study
Journal of Molecular Liquids (2020)
Effects of cationic concentration on controlling the interlayer spacings for highly effective ion rejection via graphene oxide membranes
Chemical Communications (2020)