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Rapid Fabrication of Tendon-inspired Ultrastrong, Water-rich Hydrogel Fibers: Synergistic Engineering of Cyano-p-aramid Nanofibers and Poly(vinyl alcohol)
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    Rapid Fabrication of Tendon-inspired Ultrastrong, Water-rich Hydrogel Fibers: Synergistic Engineering of Cyano-p-aramid Nanofibers and Poly(vinyl alcohol)
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    • Hyo Jeong Kim
      Hyo Jeong Kim
      Department of Organic and Nano Engineering, Human-Tech Convergence Program, Hanyang University, Seoul 04763, Republic of Korea
    • Hyeonjeong Kim
      Hyeonjeong Kim
      Department of Organic and Nano Engineering, Human-Tech Convergence Program, Hanyang University, Seoul 04763, Republic of Korea
    • Yun Hyeong Choi
      Yun Hyeong Choi
      Department of Polymer Engineering, Pukyong National University, Busan 48513, Republic of Korea
    • Eun Seong Lee
      Eun Seong Lee
      Department of Biomedical Chemical Engineering, The Catholic University of Korea (CUK), Bucheon-si, Gyeonggi-do 14662, Republic of Korea
    • Yong Hyeon Kim
      Yong Hyeon Kim
      Department of Smart Green Technology Engineering, Pukyong National University, Busan 48513, Republic of Korea
    • Ga-Hyeun Lee
      Ga-Hyeun Lee
      School of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
      More by Ga-Hyeun Lee
    • Han Gi Chae
      Han Gi Chae
      School of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
      More by Han Gi Chae
    • Youngho Eom*
      Youngho Eom
      Department of Organic and Nano Engineering, Human-Tech Convergence Program, Hanyang University, Seoul 04763, Republic of Korea
      *Email: [email protected]
      More by Youngho Eom
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    ACS Nano

    Cite this: ACS Nano 2025, 19, 8, 8316–8327
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    https://doi.org/10.1021/acsnano.4c18686
    Published February 23, 2025
    Copyright © 2025 American Chemical Society

    Abstract

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    Load-bearing fibrous tissues, like tendons, have remarkable strength with high water content (∼60%) due to the anisotropic network of collagen fibers. However, the scalability of biomimetic anisotropic hydrogels is limited by time-intensive fabrication processes involving cross-linking and stretching, often spanning several hours to days. Here, we present a rapid, scalable approach for fabricating tendon-mimetic hydrogel fibers within 1 min using the synergistic engineering of cyano-p-aramid nanofibers (CY-ANFs) and poly(vinyl alcohol) (PVA). Through continuous air-gap spinning, the formation of the anisotropic CY-ANF network drives instant gelation, producing hundreds of meters of hydrogel fibers without additional gelation treatment. From the perspective of properties, the hydrophilic PVA matrix affords flexibility, while the hydrophobic CY-ANF network provides a nonswelling feature and load-bearing ability, resulting in ultrastrong, water-rich hydrogel fibers. These hydrogel fibers exhibit a water content exceeding 80 wt %, along with exceptional strength (∼17.9 MPa), surpassing the mechanical properties of natural tendons (strength and modulus of approximately 10 and 100 MPa, respectively). Lengthy hydrogel fibers are integrated into larger-sized fabrics by knitting or weaving while also possessing strain-sensing capabilities. With excellent biocompatibility, these hydrogel fibers are promising candidates for artificial fibrous tissues and various biotechnological applications.

    Copyright © 2025 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsnano.4c18686.

    • Photographs of CY-ANF solution, rheology, FTIR spectra, 2D COS analysis, mechanical cyclic tests, OM, 2D WAXS, SEM, strain sensing data, in vitro cell viability tests, and properties of commercial-grade surgical sutures. Tables of properties of P/CY-ANF hydrogel fibers, solubility parameters, and osmotic and elastic pressures (PDF)

    • Video of the spinning process and stretchability (MP4)

    • Video of the hydrogel fiber demonstrating that it is soft enough to rapidly adapt to the physical deformation of human body motion (MP4)

    • Video of the hydrogel fabric demonstrating that it is soft enough to rapidly adapt to the physical deformation of human body motion (MP4)

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    ACS Nano

    Cite this: ACS Nano 2025, 19, 8, 8316–8327
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsnano.4c18686
    Published February 23, 2025
    Copyright © 2025 American Chemical Society

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