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

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...

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Main Authors: Shaoning Zhang, Dayong Ren, Qiaoyu Zhao, Min Peng, Xia Wang, Zhitao Zhang, Wei Liu, Fuqiang Huang
Format: Article
Language:English
Published: Nature Portfolio 2025-03-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-57692-y
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author Shaoning Zhang
Dayong Ren
Qiaoyu Zhao
Min Peng
Xia Wang
Zhitao Zhang
Wei Liu
Fuqiang Huang
author_facet Shaoning Zhang
Dayong Ren
Qiaoyu Zhao
Min Peng
Xia Wang
Zhitao Zhang
Wei Liu
Fuqiang Huang
author_sort Shaoning Zhang
collection DOAJ
description 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.
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spelling doaj-art-b344cb4730394f2ea1a7830ee37b8acf2025-08-20T02:56:09ZengNature PortfolioNature Communications2041-17232025-03-0116111110.1038/s41467-025-57692-yObservation of topological hydrogen-bonding domains in physical hydrogel for excellent self-healing and elasticityShaoning Zhang0Dayong Ren1Qiaoyu Zhao2Min Peng3Xia Wang4Zhitao Zhang5Wei Liu6Fuqiang Huang7State Key Lab of Metal Matrix Composites, School of Materials Science and Engineering and Zhangjiang Institute for Advanced Study, Shanghai Jiao Tong UniversityState Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of SciencesState Key Laboratory of Molecular Biology, Shanghai Institute of Biochemistry and Cell Biology, Center for Excellence in Molecular Cell Science, University of Chinese Academy of Sciences, Chinese Academy of SciencesSchool of Physical Science and Technology, ShanghaiTech UniversitySchool of Physical Science and Technology, ShanghaiTech UniversityState Key Lab of Metal Matrix Composites, School of Materials Science and Engineering and Zhangjiang Institute for Advanced Study, Shanghai Jiao Tong UniversitySchool of Physical Science and Technology, ShanghaiTech UniversityState Key Lab of Metal Matrix Composites, School of Materials Science and Engineering and Zhangjiang Institute for Advanced Study, Shanghai Jiao Tong UniversityAbstract 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.https://doi.org/10.1038/s41467-025-57692-y
spellingShingle Shaoning Zhang
Dayong Ren
Qiaoyu Zhao
Min Peng
Xia Wang
Zhitao Zhang
Wei Liu
Fuqiang Huang
Observation of topological hydrogen-bonding domains in physical hydrogel for excellent self-healing and elasticity
Nature Communications
title Observation of topological hydrogen-bonding domains in physical hydrogel for excellent self-healing and elasticity
title_full Observation of topological hydrogen-bonding domains in physical hydrogel for excellent self-healing and elasticity
title_fullStr Observation of topological hydrogen-bonding domains in physical hydrogel for excellent self-healing and elasticity
title_full_unstemmed Observation of topological hydrogen-bonding domains in physical hydrogel for excellent self-healing and elasticity
title_short Observation of topological hydrogen-bonding domains in physical hydrogel for excellent self-healing and elasticity
title_sort observation of topological hydrogen bonding domains in physical hydrogel for excellent self healing and elasticity
url https://doi.org/10.1038/s41467-025-57692-y
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