Strain-induced crumpling of graphene oxide to achieve fast extraction of H2, CO2

3 months ago 2

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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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).

Author information

Author notes

  1. These authors contributed equally: Pengxiang Zhang, Qian Wang.

Authors and Affiliations

  1. Institute for Functional Intelligent Materials, National University of Singapore, Singapore, Singapore

    Pengxiang Zhang, Qian Wang, Yixin Zhang, Mo Lin, Xin Zhou, Andrey Ustyuzhanin, Musen Chen, Maxim Trubyanov, Kostya S. Novoselov & Daria V. Andreeva

  2. Department of Materials Science and Engineering, National University of Singapore, Singapore, Singapore

    Pengxiang Zhang, Qian Wang, Yixin Zhang, Mo Lin, Kostya S. Novoselov & Daria V. Andreeva

  3. Missouri University of Science and Technology, Rolla, MO, USA

    Ashish David

  4. Constructor Knowledge Labs, Bremen, Germany

    Andrey Ustyuzhanin

  5. Constructor University, Bremen, Germany

    Andrey Ustyuzhanin

  6. Institute for Molecules and Materials, Radboud University, Nijmegen, the Netherlands

    Mikhail I. Katsnelson

Authors

  1. Pengxiang Zhang
  2. Qian Wang
  3. Yixin Zhang
  4. Mo Lin
  5. Xin Zhou
  6. Ashish David
  7. Andrey Ustyuzhanin
  8. Musen Chen
  9. Mikhail I. Katsnelson
  10. Maxim Trubyanov
  11. Kostya S. Novoselov
  12. Daria V. Andreeva

Contributions

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.

Corresponding author

Correspondence to Daria V. Andreeva.

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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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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. (2025). https://doi.org/10.1038/s41565-025-01971-8

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  • Received: 04 September 2024

  • Accepted: 05 June 2025

  • Published: 14 July 2025

  • DOI: https://doi.org/10.1038/s41565-025-01971-8

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