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

Author

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  • Mutian Hua

    (University of California, Los Angeles)

  • Shuwang Wu

    (University of California, Los Angeles
    Shanghai Jiao Tong University)

  • 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)

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.

Suggested Citation

  • Mutian Hua & Shuwang Wu & Yanfei Ma & Yusen Zhao & Zilin Chen & Imri Frenkel & Joseph Strzalka & Hua Zhou & Xinyuan Zhu & Ximin He, 2021. "Strong tough hydrogels via the synergy of freeze-casting and salting out," Nature, Nature, vol. 590(7847), pages 594-599, February.
  • Handle: RePEc:nat:nature:v:590:y:2021:i:7847:d:10.1038_s41586-021-03212-z
    DOI: 10.1038/s41586-021-03212-z
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    Cited by:

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    16. Feipeng Chen & Xiufeng Li & Yafeng Yu & Qingchuan Li & Haisong Lin & Lizhi Xu & Ho Cheung Shum, 2023. "Phase-separation facilitated one-step fabrication of multiscale heterogeneous two-aqueous-phase gel," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
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    20. Shuzhen Yan & Kaiming Hu & Shuai Chen & Tiantian Li & Wenming Zhang & Jie Yin & Xuesong Jiang, 2022. "Photo-induced stress relaxation in reconfigurable disulfide-crosslinked supramolecular films visualized by dynamic wrinkling," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
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