Abstract
Graphene oxide (GO) membranes offer high selectivity and energy-efficient gas separation. However, their dense, layered structure and tortuous diffusion paths limit permeability, posing a barrier to industrial use. Here we present a method to enhance selectivity and permeability, maintaining the structural stability of such membranes. With an industrially friendly manufacturing method, we produce crumpled GO membranes with gas diffusion pathways controlled by a multidomain structure. These membranes achieve H2 permeability of approximately 2.1 × 104 barrer, significantly surpassing the permeability of flat lamellar GO membranes, which is below 100 barrer. Its H2/CO2 selectivity of 91 outperforms current membrane technologies. In addition, the crumpled membranes demonstrate stability under harsh conditions (−20 °C, 96% relative humidity), a critical requirement for practical applications. This work addresses the long-standing permeability–selectivity trade-off and establishes a robust, scalable platform for integrating two-dimensional materials into membrane technology for real-world applications.
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Data availability
All data supporting the findings of this study are available within the article and its Supplementary Information. Additional raw data are available from the corresponding author upon reasonable request.
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Acknowledgements
This research is supported by the Ministry of Education, Singapore, under its Research Centre of Excellence award to the Institute for Functional Intelligent Materials (I-FIM, project no. EDUNC-33-18-279V12). We thank C. Wong from KEYENCE SINGAPORE PTE LTD. for his assistance with spatial microscopy of cGO membranes using the VHX-7000 digital microscope. A.U. acknowledges funding from the Materials Generative Design and Testing Framework (MAT-GDT) programme at A*STAR, provided through the AME Programmatic Fund (grant no. M24N4b0034). K.S.N. acknowledges support from the National Research Foundation, Singapore under its AI Singapore Programme (AISG award no. AISG3-RP-2022-028) and from the Royal Society (UK, grant no. RSRP\R\190000).
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D.V.A. conceived and designed the study. P.Z., Q.W., Y.Z., M.L., X.Z., M.C. and M.T. carried out the experiments. P.Z., M.T., A.D. and A.U. performed the data collection and analysis. P.Z., Q.W., M.T., M.I.K., K.S.N. and D.V.A. contributed to the development of the mechanochemical approach. P.Z., M.T., M.I.K., K.S.N. and D.V.A. wrote the paper with input from all authors. D.V.A. supervised the project and provided overall guidance. All authors discussed the results and contributed to the final paper.
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Nature Nanotechnology thanks Haiqing Lin, Weishen Yang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
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Supplementary Figs. 1–25, Tables 1–3 and discussion.
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Formation of cGO membranes during thermal shrinkage of polymer support.
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Zhang, P., Wang, Q., Zhang, Y. et al. Strain-induced crumpling of graphene oxide lamellas to achieve fast and selective transport of H2 and CO2. Nat. Nanotechnol. 20, 1254–1261 (2025). https://doi.org/10.1038/s41565-025-01971-8
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DOI: https://doi.org/10.1038/s41565-025-01971-8
