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Observation of topological hydrogen-bonding domains in physical hydrogel for excellent self-healing and elasticity

Author

Listed:
  • Shaoning Zhang

    (Shanghai Jiao Tong University
    ShanghaiTech University
    Chinese Academy of Sciences)

  • Dayong Ren

    (Chinese Academy of Sciences)

  • Qiaoyu Zhao

    (Chinese Academy of Sciences)

  • Min Peng

    (ShanghaiTech University)

  • Xia Wang

    (ShanghaiTech University)

  • Zhitao Zhang

    (Shanghai Jiao Tong University)

  • Wei Liu

    (ShanghaiTech University)

  • Fuqiang Huang

    (Shanghai Jiao Tong University)

Abstract

Physical hydrogels, three-dimensional polymer networks with reversible cross-linking, have been widely used in many developments throughout the history of mankind. However, physical hydrogels face significant challenges in applications due to wound rupture and low elasticity. Some self-heal wounds with strong ionic bond throughout the network but struggle to immediately recover during cyclic operation. In light of this, a strategy that achieves both self-healing and elasticity has been developed through the construction of topological hydrogen-bonding domains. These domains are formed by entangled button-knot nanoscale colloids of polyacrylic-acid (PAA) with an ultra-high molecular weight up to 240,000, further guiding the polymerization of polyacrylamide to reinforce the hydrogel network. The key for such colloids is the self-assembly of PAA fibers, approximately 4 nm in diameter, and the interconnecting PAA colloids possess high strength, simultaneously acting as elastic scaffold and reversibly cross-linking near wounds. The hydrogel completely recovers mechanical properties within 5 h at room temperature and consistently maintains >85% toughness in cyclic loading. After swelling, the hydrogel has 96.1 wt% of water content and zero residual strain during cycling. Such physical hydrogel not only provides a model system for the microstructural engineering of hydrogels but also broadens the scope of potential applications.

Suggested Citation

  • Shaoning Zhang & Dayong Ren & Qiaoyu Zhao & Min Peng & Xia Wang & Zhitao Zhang & Wei Liu & Fuqiang Huang, 2025. "Observation of topological hydrogen-bonding domains in physical hydrogel for excellent self-healing and elasticity," Nature Communications, Nature, vol. 16(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-57692-y
    DOI: 10.1038/s41467-025-57692-y
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    References listed on IDEAS

    as
    1. Wei Zhang & Baohu Wu & Shengtong Sun & Peiyi Wu, 2021. "Skin-like mechanoresponsive self-healing ionic elastomer from supramolecular zwitterionic network," Nature Communications, Nature, vol. 12(1), pages 1-12, December.
    2. Jeong-Yun Sun & Xuanhe Zhao & Widusha R. K. Illeperuma & Ovijit Chaudhuri & Kyu Hwan Oh & David J. Mooney & Joost J. Vlassak & Zhigang Suo, 2012. "Highly stretchable and tough hydrogels," Nature, Nature, vol. 489(7414), pages 133-136, September.
    3. Haili Qin & Tan Zhang & Na Li & Huai-Ping Cong & Shu-Hong Yu, 2019. "Anisotropic and self-healing hydrogels with multi-responsive actuating capability," Nature Communications, Nature, vol. 10(1), pages 1-11, December.
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