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Graphene oxide bulk material reinforced by heterophase platelets with multiscale interface crosslinking

Nature Materials volume 21, pages 1121–1129 (2022)Cite this article

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Abstract

Graphene oxide (GO) and reduced GO possess robust mechanical, electrical and chemical properties. Their nanocomposites have been extensively explored for applications in diverse fields. However, due to the high flexibility and weak interlayer interactions of GO nanosheets, the flexural mechanical properties of GO-based composites, especially in bulk materials, are largely constrained, which hinders their performance in practical applications. Here, inspired by the amorphous/crystalline feature of the heterophase within nacreous platelets, we present a centimetre-sized, GO-based bulk material consisting of building blocks of GO and amorphous/crystalline leaf-like MnO2 hexagon nanosheets adhered together with polymer-based crosslinkers. These building blocks are stacked and hot-pressed with further crosslinking between the layers to form a GO/MnO2-based layered (GML) bulk material. The resultant GML bulk material exhibits a flexural strength of 231.2 MPa. Moreover, the material exhibits sufficient fracture toughness and strong impact resistance while being light in weight. Experimental and numerical analyses indicate that the ordered heterophase structure and synergetic crosslinking interactions across multiscale interfaces lead to the superior mechanical properties of the material. These results are expected to provide insights into the design of structural materials and potential applications of high-performance GO-based bulk materials in aerospace, biomedicine and electronics.

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Fig. 1: Schematic illustration of the design and assembly of GML bulk material featuring amorphous/crystalline heterophase platelets and multiscale crosslinked interfaces.
Fig. 2: Characterization of heterophase structure units, typical nanocomposite films and GML bulk material.
Fig. 3: Mechanical properties of layered nanocomposite films.
Fig. 4: Mechanical properties, sharp contact indentation, residual stress fields and microcrack deflection/crack bridging of the GML bulk material.
Fig. 5: Multiple reinforcing mechanisms acting at multiple scales simulated by MD and FE models, impact-resistant properties and comparison of mechanical performance.

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Data availability

All data supporting the findings of this study are available within the paper and its Supplementary Information. Other supporting data are available from the corresponding authors upon request.

Code availability

The codes or algorithms used to analyse the data reported in this study are available from the corresponding authors upon request.

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Acknowledgements

This research was supported by the National Natural Science Foundation of China (nos. 51532001, 21905011 and 51772011). We thank J. Huang, L. Ding and X. Liu for performing various tasks in this research. SAXS measurements were supported by Y. Liu from the Testing and Evaluation Center for High-performance Fibres at BUAA.

Author information

Author notes

  1. These authors contributed equally: Ke Chen, Xuke Tang, Binbin Jia, Cezhou Cho, Yan Wei.

Authors and Affiliations

  1. Beijing Advanced Innovation Center for Biomedical Engineering, Key Laboratory of Bio-Inspired Smart Interfacial Science and Technology of Ministry of Education, School of Chemistry, Beihang University, Beijing, China

    Ke Chen, Xuke Tang, Binbin Jia, Junyu Hou & Lin Guo

  2. Department of Chemistry, The University of Tokyo, Tokyo, Japan

    Xuke Tang, Ting-Hui Xiao & Keisuke Goda

  3. School of Aeronautic Science and Engineering, Beihang University, Beijing, China

    Cezhou Chao & Leiting Dong

  4. Department of Geriatric Dentistry, NMPA Key Laboratory for Dental Materials, National Engineering Laboratory for Digital and Material Technology of Stomatology, Beijing Laboratory of Biomedical Materials, Peking University School and Hospital of Stomatology, Peking University, Beijing, China

    Yan Wei & Xuliang Deng

  5. Institute of Technological Sciences, Wuhan University, Hubei, China

    Keisuke Goda

  6. Department of Bioengineering, University of California, Los Angeles, CA, USA

    Keisuke Goda

Authors
  1. Ke Chen
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Contributions

L.G., L.D., X.D., K.C. and X.T. conceived the project and designed experiments. K.C., X.T. and B.J. carried out the design and fabrication of the lamellar composites. X.T., K.C. and B.J. characterized all samples. X.T., J.H. and K.C. performed mechanical testing. K.C., X.T. and J.H. performed in situ tensile tests. L.D. and C.C. carried out FE simulation. X.T. and C.C. compiled the videos. L.G., K.C., X.T., L.D., C.C., X.D., Y.W., B.J., T.-H.X., Y.W. and K.G. drafted the manuscript. All authors discussed the results and commented on the manuscript.

Corresponding authors

Correspondence to Leiting Dong, Xuliang Deng or Lin Guo.

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The authors declare no competing interests.

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Nature Materials thanks Lars Berglund 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 materials, preparation and characterization methods, Figs. 1–31, Discussion and Tables 1–7.

Supplementary Video 1

Evolution process of the Von Mises stress nephogram of the nanoscale heterophase reinforcing structure under uniaxial tension mode.

Supplementary Video 2

Evolution process of the Von Mises stress nephogram of the nanoscale heterophase reinforcing structure under three-point bending mode.

Supplementary Video 3

Evolution process of the Von Mises stress nephogram of the lamellar composite structure model under three-point bending mode.

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Chen, K., Tang, X., Jia, B. et al. Graphene oxide bulk material reinforced by heterophase platelets with multiscale interface crosslinking. Nat. Mater. 21, 1121–1129 (2022). https://doi.org/10.1038/s41563-022-01292-4

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