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Investigating the Thermodynamics Underlying Monosaccharide-Mediated Collagen Polymerization for Materials Design

  • Cassandra L. Martin
    Cassandra L. Martin
    Department of Chemistry and Chemical Biology, Northeastern University, Boston, Massachusetts 02115, United States
  • Michael R. Bergman
    Michael R. Bergman
    Department of Chemistry and Chemical Biology, Northeastern University, Boston, Massachusetts 02115, United States
  • Patrick A. Sullivan
    Patrick A. Sullivan
    Department of Chemistry and Chemical Biology, Northeastern University, Boston, Massachusetts 02115, United States
  • , and 
  • Leila F. Deravi*
    Leila F. Deravi
    Department of Chemistry and Chemical Biology, Northeastern University, Boston, Massachusetts 02115, United States
    *Email: [email protected]
Cite this: Chem. Mater. 2022, 34, 7, 3099–3108
Publication Date (Web):March 24, 2022
https://doi.org/10.1021/acs.chemmater.1c04153
Copyright © 2022 American Chemical Society

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    Abstract

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    The use and incorporation of type I collagen (COL) in biomaterials and regenerative medicine have remained challenging due to COL’s ability to spontaneously polymerize at physiological pH in vitro. Previous work has shown that the addition of monosaccharides can delay COL polymerization and increase its solubility under neutral conditions by three orders of magnitude─two features that enable structure retention and integration into pre-existing fibrous networks. We expand on these findings and describe the thermodynamic effects of these monosaccharides on the growth phase of COL polymerization. We derive van’t Hoff plots for each experimental condition and use these data to support an indirect mechanism for delayed COL assembly profiles based on solvent ordering. We observe that the presence of monosaccharides in a COL solution neither altered nor permanently inhibited the formation of COL fibrils. Finally, we demonstrate the utility of our findings through a proof-of-concept study which showed how the presence of these monosaccharides aided in the delivery of a high (2 mg/mL) concentration of neutralized, monomeric COL into simple patterns without disrupting COL structure formation. Our findings support the application of entropy-regulating systems such as monosaccharides in manipulating the dynamics of some self-assembling proteins to aid in biomaterials design.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.chemmater.1c04153.

    • Analysis of the rate order of COL polymerization; turbidimetric assays at varying monosaccharide concentrations and temperatures; COL controls in the absence of monosaccharides; SDS-PAGE gel results of the COL supernatant; DLS results for COL polymerization; effect of D2O on the COL assembly kinetics; and thermal stability analysis of COL fibrils with and without Gal (PDF)

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