A strategy for tough and fatigue-resistant hydrogels via loose cross-linking and dense dehydration-induced entanglements

Danming Zhong, Zhicheng Wang, Junwei Xu, Junjie Liu, Rui Xiao, Shaoxing Qu () and Wei Yang
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Danming Zhong: Zhejiang University
Zhicheng Wang: Zhejiang University
Junwei Xu: Zhejiang University
Junjie Liu: Southwest Jiaotong University
Rui Xiao: Zhejiang University
Shaoxing Qu: Zhejiang University
Wei Yang: Zhejiang University

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract Outstanding overall mechanical properties are essential for the successful utilization of hydrogels in advanced applications such as human-machine interfaces and soft robotics. However, conventional hydrogels suffer from fracture toughness-stiffness conflict and fatigue threshold-stiffness conflict, limiting their applicability. Simultaneously enhancing the fracture toughness, fatigue threshold, and stiffness of hydrogels, especially within a homogeneous single network structure, has proven to be a formidable challenge. In this work, we overcome this challenge through the design of a loosely cross-linked hydrogel with slight dehydration. Experimental results reveal that the slightly-dehydrated, loosely cross-linked polyacrylamide hydrogel, with an original/current water content of 87%/70%, exhibits improved mechanical properties, which is primarily attributed to the synergy between the long-chain structure and the dense dehydration-induced entanglements. Importantly, the creation of these microstructures does not require intricate design or processing. This simple approach holds significant potential for hydrogel applications where excellent anti-fracture and fatigue-resistant properties are necessary.

Date: 2024
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DOI: 10.1038/s41467-024-50364-3

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