Strong tough hydrogels via the synergy of freeze-casting and salting out

Mutian Hua, Shuwang Wu, Yanfei Ma, Yusen Zhao, Zilin Chen, Imri Frenkel, Joseph Strzalka, Hua Zhou, Xinyuan Zhu and Ximin He ()
Additional contact information
Mutian Hua: University of California, Los Angeles
Shuwang Wu: University of California, Los Angeles
Yanfei Ma: University of California, Los Angeles
Yusen Zhao: University of California, Los Angeles
Zilin Chen: University of California, Los Angeles
Imri Frenkel: University of California, Los Angeles
Joseph Strzalka: Argonne National Laboratory
Hua Zhou: Argonne National Laboratory
Xinyuan Zhu: Shanghai Jiao Tong University
Ximin He: University of California, Los Angeles

Nature, 2021, vol. 590, issue 7847, 594-599

Abstract: Abstract Natural load-bearing materials such as tendons have a high water content of about 70 per cent but are still strong and tough, even when used for over one million cycles per year, owing to the hierarchical assembly of anisotropic structures across multiple length scales1. Synthetic hydrogels have been created using methods such as electro-spinning2, extrusion3, compositing4,5, freeze-casting6,7, self-assembly8 and mechanical stretching9,10 for improved mechanical performance. However, in contrast to tendons, many hydrogels with the same high water content do not show high strength, toughness or fatigue resistance. Here we present a strategy to produce a multi-length-scale hierarchical hydrogel architecture using a freezing-assisted salting-out treatment. The produced poly(vinyl alcohol) hydrogels are highly anisotropic, comprising micrometre-scale honeycomb-like pore walls, which in turn comprise interconnected nanofibril meshes. These hydrogels have a water content of 70–95 per cent and properties that compare favourably to those of other tough hydrogels and even natural tendons; for example, an ultimate stress of 23.5 ± 2.7 megapascals, strain levels of 2,900 ± 450 per cent, toughness of 210 ± 13 megajoules per cubic metre, fracture energy of 170 ± 8 kilojoules per square metre and a fatigue threshold of 10.5 ± 1.3 kilojoules per square metre. The presented strategy is generalizable to other polymers, and could expand the applicability of structural hydrogels to conditions involving more demanding mechanical loading.

Date: 2021
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DOI: 10.1038/s41586-021-03212-z

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