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Genetically Engineered Protein-Based Bioadhesives with Programmable Material Properties
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    Biological and Medical Applications of Materials and Interfaces

    Genetically Engineered Protein-Based Bioadhesives with Programmable Material Properties
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    • Juya Jeon
      Juya Jeon
      Department of Energy, Environmental & Chemical Engineering, Washington University in St. Louis, One Brookings Drive, Saint Louis, Missouri 63130, United States
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    • Kok Zhi Lee
      Kok Zhi Lee
      Department of Energy, Environmental & Chemical Engineering, Washington University in St. Louis, One Brookings Drive, Saint Louis, Missouri 63130, United States
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    • Xiaolu Zhang
      Xiaolu Zhang
      Department of Energy, Environmental & Chemical Engineering, Washington University in St. Louis, One Brookings Drive, Saint Louis, Missouri 63130, United States
      More by Xiaolu Zhang
    • John Jaeger
      John Jaeger
      Department of Energy, Environmental & Chemical Engineering, Washington University in St. Louis, One Brookings Drive, Saint Louis, Missouri 63130, United States
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    • Eugene Kim
      Eugene Kim
      Department of Energy, Environmental & Chemical Engineering, Washington University in St. Louis, One Brookings Drive, Saint Louis, Missouri 63130, United States
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    • Jingyao Li
      Jingyao Li
      Department of Energy, Environmental & Chemical Engineering, Washington University in St. Louis, One Brookings Drive, Saint Louis, Missouri 63130, United States
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    • Larisa Belaygorod
      Larisa Belaygorod
      Department of Surgery, Section of Vascular Surgery, Washington University of Medicine in St. Louis, 660 South Euclid Avenue, Saint Louis, Missouri 63110, United States
    • Batool Arif
      Batool Arif
      Department of Surgery, Section of Vascular Surgery, Washington University of Medicine in St. Louis, 660 South Euclid Avenue, Saint Louis, Missouri 63110, United States
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    • Guy M. Genin
      Guy M. Genin
      NSF Science and Technology Center for Engineering MechanoBiology, Department of Mechanical Engineering & Materials Science, Washington University in St. Louis, One Brookings Drive, Saint Louis, Missouri 63130, United States
      Institute of Materials Science and Engineering, Washington University in St. Louis, One Brookings Drive, Saint Louis, Missouri 63130, United States
      Division of Biological & Biomedical Sciences, Washington University in St. Louis, One Brookings Drive, Saint Louis, Missouri 63130, United States
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    • Marcus B. Foston
      Marcus B. Foston
      Department of Energy, Environmental & Chemical Engineering, Washington University in St. Louis, One Brookings Drive, Saint Louis, Missouri 63130, United States
    • Mohamed A. Zayed
      Mohamed A. Zayed
      Department of Surgery, Section of Vascular Surgery, Washington University of Medicine in St. Louis, 660 South Euclid Avenue, Saint Louis, Missouri 63110, United States
      Department of Radiology, Washington University of Medicine in St. Louis, 660 South Euclid Avenue, Saint Louis, Missouri 63110, United States
      Division of Molecular Cell Biology, Washington University of Medicine in St. Louis, 660 South Euclid Avenue, Saint Louis, Missouri 63110, United States
      Division of Molecular Cell Biology, Washington University of Medicine in St. Louis, 660 South Euclid Avenue, Saint Louis, Missouri 63110, United States
      Veterans Affairs St. Louis Health Care System, 915 North Grand Boulevard, St. Louis, Missouri 63106, United States
    • Fuzhong Zhang*
      Fuzhong Zhang
      Department of Energy, Environmental & Chemical Engineering, Washington University in St. Louis, One Brookings Drive, Saint Louis, Missouri 63130, United States
      Institute of Materials Science and Engineering, Washington University in St. Louis, One Brookings Drive, Saint Louis, Missouri 63130, United States
      Division of Biological & Biomedical Sciences, Washington University in St. Louis, One Brookings Drive, Saint Louis, Missouri 63130, United States
      *Email: [email protected]. Tel.: +1 (314) 935-7671. Fax: +1 (314) 935-7211.
    Other Access OptionsSupporting Information (1)

    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2023, 15, 49, 56786–56795
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    https://doi.org/10.1021/acsami.3c12919
    Published December 1, 2023
    Copyright © 2023 American Chemical Society

    Abstract

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    Silk-amyloid-mussel foot protein (SAM) hydrogels made from recombinant fusion proteins containing β-amyloid peptide, spider silk domain, and mussel foot protein (Mfp) are attractive bioadhesives as they display a unique combination of tunability, biocompatibility, bioabsorbability, strong cohesion, and underwater adhesion to a wide range of biological surfaces. To design tunable SAM hydrogels for tailored surgical repair applications, an understanding of the relationships between protein sequence and hydrogel properties is imperative. Here, we fabricated SAM hydrogels using fusion proteins of varying lengths of silk-amyloid repeats and Mfps to characterize their structure and properties. We found that increasing silk-amyloid repeats enhanced the hydrogel’s β-sheet content (r = 0.74), leading to higher cohesive strength and toughness. Additionally, increasing the Mfp length beyond the half-length of the full Mfp sequence (1/2 Mfp) decreased the β-sheet content (r = −0.47), but increased hydrogel surface adhesion. Among different variants, the hydrogel made of 16xKLV-2Mfp displayed a high ultimate strength of 3.0 ± 0.3 MPa, an ultimate strain of 664 ± 119%, and an attractive underwater adhesivity of 416 ± 20 kPa to porcine skin. Collectively, the sequence-structure–property relationships learned from this study will be useful to guide the design of future protein adhesives with tunable characteristics for tailored surgical applications.

    Copyright © 2023 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/acsami.3c12919.

    • Sequence information, mechanical properties, adhesion properties, and hysteresis curves (PDF)

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    This article is cited by 2 publications.

    1. Aliakbar Jafari, Ahmed Al‐Ostaz, Sasan Nouranian. Recent Advances in Multifunctional Naturally Derived Bioadhesives for Tissue Engineering and Wound Management. Polymers for Advanced Technologies 2024, 35 (12) https://doi.org/10.1002/pat.70009
    2. Shri Venkatesh Subramani, Jingyao Li, Kok Zhi Lee, Natalie Fisher, Fuzhong Zhang. Blending recombinant amyloid silk proteins generates composite fibers with tunable mechanical properties. Materials Advances 2024, 5 (8) , 3506-3516. https://doi.org/10.1039/D3MA01056B

    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2023, 15, 49, 56786–56795
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.3c12919
    Published December 1, 2023
    Copyright © 2023 American Chemical Society

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