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Spatiotemporally-regulated multienzymatic polymerization endows hydrogel continuous gradient and spontaneous actuation

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Abstract

There are several natural materials which have evolved functional gradients, ingeniously attaining maximal efficacy from limited components. Herein, we utilized the spatiotemporal distribution of initiator acetylacetone to regulate the multienzyme polymerization and fabricate a chitosan-polymer hydrogel. The temporal priority order of acetylacetone was higher than phenol-modified chitosan by density functional theory calculation. The acetylacetone within the gelatin could gradually diffuse spatially into the chitosan hydrogel to fabricate the composite hydrogel with gradient network structure. The gradient hydrogel possessed a transferring topography from the two-dimensional pattern. A continuously decreased modulus along with acetylacetone diffusion was confirmed by atomic force microscope-based force mapping experiment. The water-retaining ability of various regions was confirmed by low-field nuclear magnetic resonance (NMR) and thermogravimetric analysis (TG) analysis, which led to the spontaneous actuation of gradient hydrogel with maximum 1821°/h curling speed and 227° curling angle. Consequently, the promising gradient hydrogels could be applied as intelligent actuators and flexible robots.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (51873156, 51773155) and the National Key Research and Development Program (2016YFA0100800).

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Authors and Affiliations

  1. School of Chemical Science and Engineering, Tongji University, Shanghai, 200092, China

    Saiji Shen, Chu Wu, Yinghui Shang, Hongdou Shen, Yue Liao, Yuting Guo, Min Hu, Xia Wang & Qigang Wang

  2. College of Electronics and Information Engineering, Tongji University, Shanghai, 201804, China

    Gang Li

Authors
  1. Saiji Shen
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  2. Chu Wu
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  3. Yinghui Shang
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  4. Hongdou Shen
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  5. Yue Liao
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  6. Yuting Guo
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  7. Min Hu
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  8. Xia Wang
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  9. Gang Li
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  10. Qigang Wang
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Corresponding authors

Correspondence to Gang Li or Qigang Wang.

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Conflict of interest The authors declare no conflict of interest.

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Supporting information The supporting information is available online at http://chem.scichina.com and http://link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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Shen, S., Wu, C., Shang, Y. et al. Spatiotemporally-regulated multienzymatic polymerization endows hydrogel continuous gradient and spontaneous actuation. Sci. China Chem. 65, 153–161 (2022). https://doi.org/10.1007/s11426-021-1107-8

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  • DOI: https://doi.org/10.1007/s11426-021-1107-8

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