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High-strength scalable graphene sheets by freezing stretch-induced alignment

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Efforts to obtain high-strength graphene sheets by near-room-temperature assembly have been frustrated by the misalignment of graphene layers, which degrades mechanical properties. While in-plane stretching can decrease this misalignment, it reappears when releasing the stretch. Here we use covalent and π–π inter-platelet bridging to permanently freeze stretch-induced alignment of graphene sheets, and thereby increase isotropic in-plane sheet strength to 1.55 GPa, in combination with a high Young’s modulus, electrical conductivity and weight-normalized shielding efficiency. Moreover, the stretch-bridged graphene sheets are scalable and can be easily bonded together using a commercial resin without appreciably decreasing the performance, which establishes the potential for practical applications.

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Fig. 1: Schematic illustration of the fabrication process and the structure of a SB-BS-rGO sheet.
Fig. 2: Structural characterization of a rGO sheet and a SB-BS-rGO sheet.
Fig. 3: Properties of a rGO sheet and a SB-BS-rGO sheet.
Fig. 4: Raman, thermal expansion, stress relaxation and X-ray diffraction data for a rGO sheet and a SB-BS-rGO sheet.
Fig. 5: Mechanical and electrical properties of overlapped and laminated SB-BS-rGO sheets and SB-BS-rGO (DB) sheets made by DB casting.

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The data that support the findings of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

This work was supported by the Excellent Young Scientist Foundation of NSFC (grant no. 51522301), the National Natural Science Foundation of China (grant nos 22075009, 51961130388, 21875010, 51103004 and 52003011), Newton Advanced Fellowship (grant no. NAF\R1\191235), Beijing Natural Science Foundation (JQ19006), the National Postdoctoral Programme for Innovative Talents (BX20200038), the China Postdoctoral Science Foundation (2019M660387), the 111 Project (B14009), the Postdoctoral Research Program on Innovative Practice in Jiangmen and Excellent Sino-Foreign Young Scientist Exchange Program of CAST. Support at the University of Texas at Dallas was provided by the Air Force Office of Scientific Research grant no. FA9550-18-1-0510, the Robert A. Welch Foundation grant no. AT-0029 and National Science Award no. CMMI-1636306. We thank the High Performance Computing Platform at Beihang University for help with some simulation experiments.

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Authors

Contributions

Q.C. supervised the project and Q.C. and R.H.B. conceived it. S. Wan performed the experiments and characterizations. S. Wang and Z.X. carried out the MD simulations and theoretical analysis. S. Wan and Y.C. carried out in situ Raman testing and analysed the data. S. Wan, Y.C., S.F., L.J., R.H.B. and Q.C. cowrote the manuscript. All authors discussed the results and commented on the manuscript.

Corresponding authors

Correspondence to Ray H. Baughman or Qunfeng Cheng.

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The authors declare no competing interests.

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Peer review information Nature Materials thanks Jie Lian 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 Methods, Notes 1–7, Figs. 1–32, Tables 1–12 and references.

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Wan, S., Chen, Y., Fang, S. et al. High-strength scalable graphene sheets by freezing stretch-induced alignment. Nat. Mater. 20, 624–631 (2021). https://doi.org/10.1038/s41563-020-00892-2

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