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Ultrathin graphene-based membrane with precise molecular sieving and ultrafast solvent permeation

Abstract

Graphene oxide (GO) membranes continue to attract intense interest due to their unique molecular sieving properties combined with fast permeation1,2,3,4,5,6,7,8,9. However, their use is limited to aqueous solutions because GO membranes appear impermeable to organic solvents1, a phenomenon not yet fully understood. Here, we report efficient and fast filtration of organic solutions through GO laminates containing smooth two-dimensional (2D) capillaries made from large (10–20 μm) flakes. Without modification of sieving characteristics, these membranes can be made exceptionally thin, down to 10 nm, which translates into fast water and organic solvent permeation. We attribute organic solvent permeation and sieving properties to randomly distributed pinholes interconnected by short graphene channels with a width of 1 nm. With increasing membrane thickness, organic solvent permeation rates decay exponentially but water continues to permeate quickly, in agreement with previous reports1,2,3,4. The potential of ultrathin GO laminates for organic solvent nanofiltration is demonstrated by showing >99.9% rejection of small molecular weight organic dyes dissolved in methanol. Our work significantly expands possibilities for the use of GO membranes in purification and filtration technologies.

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Figure 1: Ultrathin HLGO membrane.
Figure 2: Molecular sieving and organic solvent nanofiltration through HLGO membranes.
Figure 3: Probing molecular permeation through HLGO membranes.

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Acknowledgements

This work was supported by the Royal Society, Engineering and Physical Sciences Research Council, UK (EP/K016946/1), Lloyd’s Register Foundation, and European Research Council (contract 679689). Q.Y. acknowledges support from the China Scholarship Council. We thank P. Bentley for assisting with XPS measurements, J. Waters for X-ray measurements, and K. Huang for assisting in setting up the cold trap for filtration experiments.

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R.R.N. and Y.S. designed and supervised the project. Q.Y., Y.S. and C.C prepared the samples, performed the measurements and carried out the analysis with help from R.R.N. C.T.C. and K.H. helped in sample preparation, characterization and data analysis. J.C.Z. and A.P. contributed to XPS characterization. V.G.K. and A.N.G. contributed to optical measurements. F.G., F.C.W. and A.K.G. contributed to theoretical modelling. Y.S., A.N.G., A.K.G. and R.R.N. wrote the manuscript. All authors contributed to discussions.

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Correspondence to Y. Su or R. R. Nair.

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The authors declare no competing financial interests.

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Yang, Q., Su, Y., Chi, C. et al. Ultrathin graphene-based membrane with precise molecular sieving and ultrafast solvent permeation. Nature Mater 16, 1198–1202 (2017). https://doi.org/10.1038/nmat5025

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