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Effect of Divalent Metal Cations on the Conformation, Elastic Behavior, and Controlled Release of a Photocrosslinked Protein Engineered Hydrogel
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    Effect of Divalent Metal Cations on the Conformation, Elastic Behavior, and Controlled Release of a Photocrosslinked Protein Engineered Hydrogel
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    • Yao Wang
      Yao Wang
      Department of Chemical and Biomolecular Engineering, New York University Tandon School of Engineering, Brooklyn, New York 11201, United States
      More by Yao Wang
    • Xiaole Wang
      Xiaole Wang
      Department of Chemical and Biomolecular Engineering, New York University Tandon School of Engineering, Brooklyn, New York 11201, United States
      More by Xiaole Wang
    • Jin Kim Montclare*
      Jin Kim Montclare
      Department of Chemical and Biomolecular Engineering, New York University Tandon School of Engineering, Brooklyn, New York 11201, United States
      Department of Chemistry, New York University, New York, New York 10003, United States
      Department of Biomaterials, New York University College of Dentistry, New York, New York 10010, United States
      Department of Radiology, New York University Langone Health, New York, New York 10016, United States
      *Email: [email protected]
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    ACS Applied Bio Materials

    Cite this: ACS Appl. Bio Mater. 2021, 4, 4, 3587–3597
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    https://doi.org/10.1021/acsabm.1c00091
    Published March 24, 2021
    Copyright © 2021 American Chemical Society

    Abstract

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    We investigate the effect of Zn2+, Cu2+, and Ni2+ coordination on the conformation, mechanical properties, contraction, and small-molecule drug encapsulation and release of a photocrosslinked protein-engineered hydrogel, CEC-D. The treatment of the CEC-D hydrogel with divalent metal (M2+) results in significant conformational changes where a loss in structure is observed with Zn2+, while both Cu2+ and Ni2+ induce a blueshift. The relationship of M2+ to mechanical properties illustrates a trend, while the CEC-D hydrogel in the presence of 2 mM Cu2+ reveals the highest increase in G′ to 14.4 ± 0.7 kPa followed by 9.7 ± 0.9 kPa by addition of 2 mM Zn2+, and a decrease to 1.1 ± 0.2 kPa is demonstrated in the presence of 2 mM Ni2+. A similar observation in M2+ responsiveness emerges where CEC-D hydrogels contract into a condensed state of 2.6-fold for Cu2+, 2.4-fold for Zn2+, and 1.6-fold for Ni2+. Furthermore, CEC-D hydrogels coordinated with M2+ demonstrate control over the encapsulation and release of the small molecule curcumin. The trend of release is opposite of the mechanical and contraction properties with a 70.0 ± 5.3% release with Ni2+, 64.2 ± 1.2% release with Zn2+, and 42.3 ± 11.3 release with Cu2+. Taken together, these results indicate that the CEC-D hydrogel tuned by M2+ is a promising drug delivery platform with tunable physicochemical properties.

    Copyright © 2021 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/acsabm.1c00091.

    • Rheology for the storage modulus (G′) and the loss modulus (G″) for the CEC-D hydrogel (n = 3) in water and different concentrations of M2+; storage modulus of CEC-D hydrogels (n = 3) contracted in water and different molar ratios of CuSO4, ZnSO4, and NiSO4 solutions; and sustained release profile of CCM measured as a function of time for the CEC-D hydrogel in the presence and absence of divalent metal cations fitted to the modified Gallagher–Corrigan model of drug release (PDF)

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    This article is cited by 8 publications.

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    ACS Applied Bio Materials

    Cite this: ACS Appl. Bio Mater. 2021, 4, 4, 3587–3597
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsabm.1c00091
    Published March 24, 2021
    Copyright © 2021 American Chemical Society

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