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Highly compressible glass-like supramolecular polymer networks

Abstract

Supramolecular polymer networks are non-covalently crosslinked soft materials that exhibit unique mechanical features such as self-healing, high toughness and stretchability. Previous studies have focused on optimizing such properties using fast-dissociative crosslinks (that is, for an aqueous system, dissociation rate constant kd > 10 s1). Herein, we describe non-covalent crosslinkers with slow, tuneable dissociation kinetics (kd < 1 s−1) that enable high compressibility to supramolecular polymer networks. The resultant glass-like supramolecular networks have compressive strengths up to 100 MPa with no fracture, even when compressed at 93% strain over 12 cycles of compression and relaxation. Notably, these networks show a fast, room-temperature self-recovery (< 120 s), which may be useful for the design of high-performance soft materials. Retarding the dissociation kinetics of non-covalent crosslinks through structural control enables access of such glass-like supramolecular materials, holding substantial promise in applications including soft robotics, tissue engineering and wearable bioelectronics.

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Fig. 1: Design of glass-like SPNs.
Fig. 2: Thermodynamic and kinetic properties of slow-dissociative non-covalent crosslinks.
Fig. 3: Rheological characterization of glass-like SPNs.
Fig. 4: Evaluation of compressive properties of glass-like SPNs.
Fig. 5: Demonstration of rapid self-recovery of glass-like SPNs and their application.

Data availability

Data generated and analysed during this study are provided as source data with this paper or included in the Supplementary Information. Further data are available from the corresponding authors upon request.

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Acknowledgements

O.A.S. and G.W. acknowledge the Leverhulme Trust Program Grant (Natural Materials Innovation). Z.H. acknowledges the Marie Skłodowska-Curie Fellowship (no. 845640). X.C. acknowledges Cambridge Display Technology (CDT) for financial support. D.J.W. thanks the Engineering and Physical Sciences Research Council for a PhD studentship (grant no. EP/R512461/1). We thank G.G. Malliaras for helpful discussions.

Author information

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Z.H. and O.A.S. conceived the idea. Z.H., X.C., S.J.K.O., G.W., D.J.W., J.A.M. and O.A.S. designed the experiments. Z.H. executed most of the experiments and analysed the data. X.C., S.J.K.O., G.W., D.J.W., J.L. and J.A.M. helped perform some of the experiments and data analysis. Z.H., J.A.M. and O.A.S. wrote the paper. All authors discussed the experiments, edited the paper and gave consent for this publication under the supervision of O.A.S.

Corresponding author

Correspondence to Oren A. Scherman.

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The authors declare no competing interests.

Additional information

Peer review information Nature Materials thanks Richard Hoogenboom, Rebecca Kramer-Bottiglio and Mathew Webber for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Charts 1 and 2, Figs. 1–41, Tables 1–5 and description of Videos 1–6.

Supplementary Video 1

Compressive test: 100 MPa.

Supplementary Video 2

Compressive test: 1.0 GPa.

Supplementary Video 3

Human compression demo.

Supplementary Video 4

Car-compression demo.

Supplementary Video 5

Ionic conductor demo.

Supplementary Video 6

Ball-drop demo.

Source data

Source Data Fig. 2

Source data in tables for Fig. 2 in the main text.

Source Data Fig. 3

Source data in tables for Fig. 3 in the main text.

Source Data Fig. 4

Source data in tables for Fig. 4 in the main text.

Source Data Fig. 5

Source data in tables for Fig. 5 in the main text.

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Huang, Z., Chen, X., O’Neill, S.J.K. et al. Highly compressible glass-like supramolecular polymer networks. Nat. Mater. (2021). https://doi.org/10.1038/s41563-021-01124-x

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