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Synthesis of two-dimensional ordered graphdiyne membranes for highly efficient and selective water transport

Nature Water volume 3, pages 307–318 (2025)Cite this article

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Abstract

Developing artificial membranes with stable and uniform angstrom-scale channels that can effectively reject hydrated ions is a substantial challenge but important in water desalination and energy conversion/storage applications. Achieving precise water/ions separation while maintaining high water flux requires a membrane microstructure engineered with molecular precision. This study reports the successful synthesis of ultra-thin, centimetre-scale graphdiyne (GDY) films with ordered one-dimensional (1D) channels using single-crystalline Cu (111) as the growth substrate and demonstrates their exceptional performance as molecular sieves for highly efficient water/ion separation. The optimized membrane exhibits an ultra-high water/NaCl selectivity of 5.96 × 104, outperforming state-of-the-art membranes, at a water permeance of ∼32.9 mol m−2 h−1 bar−1 and a salt rejection exceeding 99.7% for small ions in seawater. Mechanism studies reveal that the hydrophobic angstrom-scale channels in GDY crystals force water molecules into a single-file configuration with 1D hydrogen bond during water permeation. The 1D water chain enables the GDY membrane to facilitate rapid (diffusion constant as high as 1.3 × 10−4 cm2 s−1) and selective proton transport via the Grotthuss mechanism. This work contributes to the development of carbon nanomaterial membranes for precise molecular sieving and biomimetic protonophores.

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Fig. 1: Synthesis and characterization of c-GDY films.
Fig. 2: Water and ion transport properties of c-GDY membranes.
Fig. 3: Mechanistic study of water transport through GDY membranes.
Fig. 4: The water transport mechanism of c-GDY membranes.

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The data supporting the findings of this study are available in the paper and its Supplementary Information. Source data are provided with this paper.

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Acknowledgements

Financial support for this work was provided by Baseline Funds (BAS/1/1375-01-01 and FCC/1/5937-05-01 to Z.L.) from King Abdullah University of Science and Technology (KAUST). Y.H. acknowledges the support from the GJYC programme of Guangzhou City (2024D03J0001).

Author information

Authors and Affiliations

  1. Division of Physical Sciences and Engineering (PSE), King Abdullah University of Science and Technology (KAUST), Thuwal, Saudi Arabia

    Jiaqiang Li, Qing Liu, Bo Tian, Xiaowei Liu, Li Cao, Guanxing Li, Xixiang Zhang & Zhiping Lai

  2. College of Energy, Soochow Institute for Energy and Materials InnovationS (SIEMIS), Jiangsu Provincial Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies, Soochow University, Suzhou, China

    Ke Zhou

  3. School of Materials Science and Engineering, Nanyang Technological University, Singapore, Singapore

    Bo Tian

  4. Division of Computer, Electrical, and Mathematical Science and Engineering, King Abdullah University of Science and Technology, Thuwal, Saudi Arabia

    Haicheng Cao

  5. School of Applied and Engineering Physics, Cornell University, Ithaca, NY, USA

    Guanxing Li

  6. Center for Electron Microscopy, South China University of Technology, Guangzhou, China

    Yu Han

  7. School of Emergent Soft Matter, South China University of Technology, Guangzhou, China

    Yu Han

  8. State Key Laboratory of Pulp and Paper Engineering, South China University of Technology, Guangzhou, China

    Yu Han

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Contributions

Z.L., Y.H. and J.L. conceived and designed the experiments. J.L. and B.T. prepared the Cu (111)/Al2O3(0001) substrate. X.Z. provided important guidelines for Cu (111) substrate preparation. J.L., Q.L., X.L. and L.C. performed the synthesis of GDY materials, characterizations and transport measurements. K.Z. performed the ab initio molecular dynamics simulations and calculation of the potential of means force. H.C. performed the electronic measurements. G.L. performed the TEM measurement. All authors were involved in the analysis and discussion of the results. Z.L., Y.H., J.L., L.C. and Q.L. wrote the paper, and all authors commented on the paper.

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Correspondence to Yu Han or Zhiping Lai.

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Nature Water thanks Jin Zhang, Junyong Zhu and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Methods, Figs. 1–53, Tables 1–6 and description of the videos.

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Supplementary Video 1 (download MP4 )

A free-standing c-GDY film floating on the water indicates good mechanical strength as its macrostructure remains integrated despite external disturbances.

Supplementary Video 2 (download MP4 )

Water molecules moving in the channels to form regular 1D chains inside the membrane.

Supplementary Video 3 (download MP4 )

Density-functional-theory-calculated diffusion of proton in GDY membrane.

Supplementary Data 1

Chembiodraw structure of Fig. 1.

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Li, J., Zhou, K., Liu, Q. et al. Synthesis of two-dimensional ordered graphdiyne membranes for highly efficient and selective water transport. Nat Water 3, 307–318 (2025). https://doi.org/10.1038/s44221-025-00397-9

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