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Graphene oxide membranes with stable porous structure for ultrafast water transport

Nature Nanotechnology volume 16, pages 337–343 (2021)Cite this article

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Abstract

The robustness of carbon nanomaterials and their potential for ultrahigh permeability has drawn substantial interest for separation processes. However, graphene oxide membranes (GOms) have demonstrated limited viability due to instabilities in their microstructure that lead to failure under cross-flow conditions and applied hydraulic pressure. Here we present a highly stable and ultrapermeable zeolitic imidazolate framework-8 (ZIF-8)-nanocrystal-hybridized GOm that is prepared by ice templating and subsequent in situ crystallization of ZIF-8 at the nanosheet edges. The selective growth of ZIF-8 in the microporous defects enlarges the interlayer spacings while also imparting mechanical integrity to the laminate framework, thus producing a stable microstructure capable of maintaining a water permeability of 60 l m−2 h−1 bar−1 (30-fold higher than GOm) for 180 h. Furthermore, the mitigation of microporous defects via ZIF-8 growth increased the permselectivity of methyl blue molecules sixfold. Low-field nuclear magnetic resonance was employed to characterize the porous structure of our membranes and confirm the tailored growth of ZIF-8. Our technique for tuning the membrane microstructure opens opportunities for developing next-generation nanofiltration membranes.

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Fig. 1: Preparation and characterization of ZIF-8@f-GOm.
Fig. 2: Pore structure of GO-based membranes and elucidation of ZIF-8 growth mechanisms.
Fig. 3: Nanofiltration performance of GO-based membranes under cross-flow conditions.
Fig. 4: Elucidation of ZIF-8@f-GOm separation mechanisms.

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Data availability

The data that support the plots within this paper and other findings of this study are available from the corresponding authors upon reasonable request.

Change history

  • 06 April 2022

    In the version of the Supplementary Information initially published online, there were two errors in presentation. In Supplementary Fig 13, the contents for captions b and f and c and e were interchanged. In Supplementary Fig. 15, the orange trace in the top panel for GOm (wet) was a duplicate a center panel trace for f-GOm (dry). The captions and the GOm (wet) trace have been corrected in the revised Supplementary Information accompanying this article. None of the above corrections impacts the conclusions or discussions in the paper.

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Acknowledgements

This work is financially supported by the National Natural Science Foundation of China (21878004 and 21576003), the Importation and Development of High-Caliber Talents Project of Beijing Municipal Institutions (CIT&TCD20170305), Beijing Municipal Natural Science Foundation co-sponsored by Beijing Natural Science Foundation Committee and Beijing Education Committee (KZ201910005001) and National Key R&D Program of China (2019YFC1806000). We also acknowledge the United States National Science Foundation Graduate Research Fellowship awarded to C.L.R. (DGE1752134).

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Authors and Affiliations

  1. Beijing Key Laboratory for Green Catalysis and Separation, College of Environmental and Energy Engineering, Beijing University of Technology, Beijing, China

    Wen-Hai Zhang, Ming-Jie Yin, Cheng-Gang Jin, Naixin Wang, Shulan Ji & Quan-Fu An

  2. Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan, China

    Qiang Zhao

  3. Department of Chemical and Environmental Engineering, Yale University, New Haven, CT, USA

    Cody L. Ritt & Menachem Elimelech

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  1. Wen-Hai Zhang
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Contributions

W.-H.Z., C.L.R., M.E. and Q.-F.A. conceived and designed the experiments. M.E. and Q.-F.A. supervised the study and experiments. W.-H.Z. and C.-G.J. conducted the membrane fabrication, characterization and performance tests. S.J. and Q.-F.A. supported all the characterizations. W.-H.Z., M.-J.Y., N.W., C.L.R. and Q.-F.A. analysed the experimental results. W.-H.Z., M.-J.Y. and Q.Z. wrote the paper. C.L.R., M.E. and Q.-F.A. revised the manuscript. All the authors discussed the results and provided comments.

Corresponding authors

Correspondence to Menachem Elimelech or Quan-Fu An.

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The authors declare no competing interests.

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Peer review information Nature Nanotechnology thanks Ho Bum Park and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–17, discussion and Tables 1–5.

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Zhang, WH., Yin, MJ., Zhao, Q. et al. Graphene oxide membranes with stable porous structure for ultrafast water transport. Nat. Nanotechnol. 16, 337–343 (2021). https://doi.org/10.1038/s41565-020-00833-9

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