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A general strategy for synthesizing biomacromolecular ionogel membranes via solvent-induced self-assembly

Nature Synthesis volume 2, pages 864–872 (2023)Cite this article

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Abstract

Two-dimensional (2D) ionogel membranes have emerged as a promising class of materials for broad applications in flexible electronics, smart robotics and artificial intelligence. However, the rapid, reliable and reproducible fabrication of ionogel membranes remains challenging due to difficult-to-control molecular behaviour. To overcome this challenge, we propose a ‘dip and peel’ strategy to exfoliate 2D ionogel membranes from a biomacromolecular gelatum (for example, a cellulose ionogel colloid) by controlling the solvent-induced supramolecular self-assembly. This strategy enables the simple and rapid fabrication of ionogel membranes with tunable shapes, controllable thicknesses, high ionic conductivity up to 14.1 mS cm−1, good stretchability exceeding 130% and excellent tandem duplication over 700 times. We further extend this strategy to fabricate different ionogel membranes from various biomacromolecules, including silk fibroin, chitosan and guar gum. Our results shed light on exploration of fundamental macromolecular interactions and provide an effective approach to prepare 2D biomacromolecular ionogel membranes with advanced functionalities.

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Fig. 1: A general solvent-induced exfoliation strategy inspired by the ‘milk-skin effect’.
Fig. 2: Preparation of the P-membranes from the bulk cellulose/[Bmim]Cl colloid.
Fig. 3: Microstructure characterizations of the P-membrane.
Fig. 4: MD simulations and spectroscopic analyses.
Fig. 5: Mechanical properties and ionic conductivity of P-membrane and demonstrations of potential application.
Fig. 6: Universality of the solvent-induced exfoliation strategy.

Data availability

All data generated or analysed during this study are available within the paper and its Supplementary Information.

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Acknowledgements

H.Y. and D.Z. acknowledge support by the National Science Fund for Distinguished Young Scholars of China (grant number 31925028) and the National Natural Science Foundation of China (grant number 32171720). G.Y. acknowledges support from the Welch Foundation F-1861, a Norman Hackerman Award in Chemical Research and a Camille Dreyfus Teacher-Scholar Award.

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Authors and Affiliations

  1. Key Laboratory of Bio-based Material Science and Technology of Ministry of Education, Northeast Forestry University, Harbin, China

    Ying Zhu, Kaiyue Cao, Suqing Zeng, Yongzhuang Liu, Wanke Cheng, Wenjing Bai, Xuanli Weng, Wenshuai Chen, Dawei Zhao & Haipeng Yu

  2. Materials Science and Engineering Program and Walker Department of Mechanical Engineering, University of Texas at Austin, Austin, TX, USA

    Youhong Guo & Guihua Yu

  3. Key Laboratory on Resources Chemicals and Materials of Ministry of Education, Shenyang University of Chemical Technology, Shenyang, China

    Geyuan Jiang & Dawei Zhao

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  1. Ying Zhu
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Contributions

G.Y., H.Y. and D.Z. supervised the project and designed the experiments. Y.Z. carried out most of the experiments. K.C., S.Z., G.J., W.C., W.B. and X.W. participated in the experiments. G.J. contributed to the analysis of MD simulations. Y.G., Y.L. and W.C. contributed to analysis of the Hansen solubility parameters. Y.Z., D.Z. and H.Y. contributed to the application of e-skin. Y.Z, Y.G., D.Z., H.Y. and G.Y. collectively wrote the paper. All authors discussed the results and commented on the manuscript.

Corresponding authors

Correspondence to Dawei Zhao, Haipeng Yu or Guihua Yu.

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The authors declare no competing interests.

Peer review

Peer review information

Nature Synthesis thanks Jian Hu, Ho Seok Park and the other, anonymous, reviewer(s) for their contribution to the peer review of this work. Primary Handling Editor: Peter Seavill, in collaboration with the Nature Synthesis team.

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Supplementary information

Supplementary Information

Supplementary Notes 1 and 2, Figs. 1–20 and Tables 1–5.

Supplementary Video 1

Solvent-induced exfoliation of P-membrane within 1 s.

Supplementary Video 2

A glass-rod-assisted transfer method to obtain a flat P-membrane.

Supplementary Video 3

Layer-by-layer peeling of the P-membranes.

Supplementary Video 4

Fabrication of a large-area P-membrane.

Supplementary Video 5

Inkjet printing the P-membrane-based flexible circuit chip.

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Zhu, Y., Guo, Y., Cao, K. et al. A general strategy for synthesizing biomacromolecular ionogel membranes via solvent-induced self-assembly. Nat. Synth 2, 864–872 (2023). https://doi.org/10.1038/s44160-023-00315-5

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