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Near-room-temperature water-mediated densification of bulk van der Waals materials from their nanosheets

Nature Materials (2024)Cite this article

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Abstract

The conventional fabrication of bulk van der Waals (vdW) materials requires a temperature above 1,000 °C to sinter from the corresponding particulates. Here we report the near-room-temperature densification (for example, ∼45 °C for 10 min) of two-dimensional nanosheets to form strong bulk materials with a porosity of <0.1%, which are mechanically stronger than the conventionally made ones. The mechanistic study shows that the water-mediated activation of van der Waals interactions accounts for the strong and dense bulk materials. Initially, water adsorbed on two-dimensional nanosheets lubricates and promotes alignment. The subsequent extrusion closes the gaps between the aligned nanosheets and densifies them into strong bulk materials. Water extrusion also generates stresses that increase with moulding temperature, and too high a temperature causes intersheet misalignment; therefore, a near-room-temperature moulding process is favoured. This technique provides an energy-efficient alternative to design a wide range of dense bulk van der Waals materials with tailored compositions and properties.

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Fig. 1: Moulding of nanosheets to prepare strong, densified bulk vdW materials.
Fig. 2: Change in mechanical properties and microstructure of bulk hBN as a function of moulding temperature.
Fig. 3: Understanding the role of water in the moulding of bulk hBN.
Fig. 4: Processability of moulded bulk hBN and its thermal properties.

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Data availability

All relevant data supporting the findings of this study are available in the Article and its Supplementary Information. All other data that support the findings of this study are available from the corresponding authors upon reasonable request. Source data are provided with this paper.

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Acknowledgements

This research was primarily supported by the National Key Research and Development Program of China (no. 2022YFA1205300 to Y.S.), the National Natural Science Foundation of China (no. 52188101 to H.-M.C. and no. 12232016 to H.W.), the Young Scientist Fund of the National Natural Science Foundation of China (no. 52102363 to J.Z.), the Scientific Research Start-up Funds of Tsinghua SIGS (QD2021026C to Y.S.), Peacock Team project (KQTD20210811090112002 to Y.S.) and Shenzhen Geim Graphene Center. F.W. acknowledges the support from the Youth Innovation Promotion Association CAS (no. 2020449). The numerical calculations were performed on the supercomputing system in the Hefei Advanced Computing Center.

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Author notes

  1. These authors contributed equally: Jiuyi Zhu, Fei Li, YuanZhen Hou.

Authors and Affiliations

  1. Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, People’s Republic of China

    Jiuyi Zhu, Fei Li, Hang Li, Dingxin Xu, Junyang Tan & Yang Su

  2. State Key Laboratory of Mesoscience and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing, People’s Republic of China

    Jiuyi Zhu

  3. CAS Key Laboratory of Mechanical Behavior and Design of Materials, Department of Modern Mechanics, University of Science and Technology of China, Hefei, People’s Republic of China

    YuanZhen Hou, HengAn Wu & FengChao Wang

  4. Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, People’s Republic of China

    Jinhong Du, Shaogang Wang & Hui-Ming Cheng

  5. School of Materials Science and Engineering, Guangdong Provincial Key Laboratory of Advanced Energy Storage Materials, South China University of Technology, Guangzhou, People’s Republic of China

    Zhengbo Liu

  6. Shenzhen Key Laboratory of Energy Materials for Carbon Neutrality, Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, People’s Republic of China

    Hui-Ming Cheng

  7. Faculty of Materials Science and Energy Engineering, Shenzhen University of Advanced Technology, Shenzhen, People’s Republic of China

    Hui-Ming Cheng

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Contributions

Y.S., H.-M.C. and J.Z. conceived the idea and supervised the project. Y.S., J.Z. and F.L. designed and performed the experiments and analysed the results. H.L. and D.X. performed the moulding of bulk graphite from rGO nanosheets. J.T. performed the transmission electron microscopy examination. J.D. helped with the compression tests. S.W. performed the nano-CT measurements; Z.L. performed the focused ion beam measurements; and Y.H., F.W. and H.W. performed the MD simulation. All authors analysed the data. Y.S., J.Z. and H.-M.C. wrote the paper with input from all authors.

Corresponding authors

Correspondence to Yang Su or Hui-Ming Cheng.

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Competing interests

J.Z., Y.S. and H.-M.C. report a Chinese patent (CN113929430A). The other authors declare no competing interests.

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Nature Materials thanks Adri Van Duin, Chong Rae Park and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Sections 1–9, Figs. 1–9, Tables 1 and 2 and Discussion.

Supplementary Video 1

Mechanically strong densified bulk hBN.

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Source Data Fig. 2

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Source Data Fig. 3

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Zhu, J., Li, F., Hou, Y. et al. Near-room-temperature water-mediated densification of bulk van der Waals materials from their nanosheets. Nat. Mater. (2024). https://doi.org/10.1038/s41563-024-01840-0

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