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

Shaoning Zhang, Dayong Ren, Qiaoyu Zhao, Min Peng, Xia Wang, Zhitao Zhang, Wei Liu () and Fuqiang Huang ()
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Shaoning Zhang: Shanghai Jiao Tong University
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

Nature Communications, 2025, vol. 16, issue 1, 1-11

Abstract: 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.

Date: 2025
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DOI: 10.1038/s41467-025-57692-y

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