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    Thermal and Structural Properties of Silk Biomaterials Plasticized by Glycerol
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    † †Department of Biomedical Engineering and §Department of Physics and Astronomy, Tufts University, Medford, Massachusetts 02155, United States
    ‡ School of Molecular Sciences and the Magnetic Resonance Research Center, Arizona State University, Tempe, Arizona 85287-1604, United States
    ∥ Department of Chemistry and Biochemistry, San Diego State University, 5500 Campanile Drive, San Diego, California 92182-1030, United States
    *E-mail: [email protected]. Tel.: +1-617-627-3251. Fax: +1-617-627-3231.
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    Biomacromolecules

    Cite this: Biomacromolecules 2016, 17, 12, 3911–3921
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    https://doi.org/10.1021/acs.biomac.6b01260
    Published November 18, 2016
    Copyright © 2016 American Chemical Society
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    Abstract

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    The molecular interactions of silk materials plasticized using glycerol were studied, as these materials provide options for biodegradable and flexible protein-based systems. Plasticizer interactions with silk were analyzed by thermal, spectroscopic, and solid-state NMR analyses. Spectroscopic analysis implied that glycerol was hydrogen bonded to the peptide matrix, but may be displaced with polar solvents. Solid-state NMR indicated that glycerol induced β-sheet formation in the dried silk materials, but not to the extent of methanol treatment. Fast scanning calorimetry suggested that β-sheet crystal formation in silk-glycerol films appeared to be less organized than in the methanol treated silk films. We propose that glycerol may be simultaneously inducing and interfering with β-sheet formation in silk materials, causing some improper folding that results in less-organized silk II structures even after the glycerol is removed. This difference, along with trace residual glycerol, allows glycerol extracted silk materials to retain more flexibility than methanol processed versions.

    Copyright © 2016 American Chemical Society

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.biomac.6b01260.

    • Expanded solid-state NMR spectra for Figure 2, as well as background DMTA data supplementing Figures 5 and 6 (PDF).

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    Cited By

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    Biomacromolecules

    Cite this: Biomacromolecules 2016, 17, 12, 3911–3921
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.biomac.6b01260
    Published November 18, 2016
    Copyright © 2016 American Chemical Society
    Request reuse permissions

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