Water-insoluble silk films with silk I structure
Open accessAbstract
Water-insoluble regenerated silk materials are normally produced by increasing the beta-sheet content (silk II). In the present study water-insoluble silk films were prepared by controlling the very slow drying of Bombyx mori silk solutions, resulting in the formation of stable films with a predominant silk I instead of silk II structure. Wide angle X-ray scattering indicated that the silk films stabilized by slow drying were mainly composed of silk I rather than silk II, while water- and methanol-annealed silk films had a higher silk II content. The silk films prepared by slow drying had a globule-like structure at the core surrounded by nano-filaments. The core region was composed of silk I and silk II, surrounded by hydrophilic nano-filaments containing random turns and alpha-helix secondary structures. The insoluble silk films prepared by slow drying had unique thermal, mechanical and degradative properties. Differential scanning calorimetry results revealed that silk I crystals had stable thermal properties up to 250 degrees C, without crystallization above the T(g), but degraded at lower temperatures than silk II structure. Compared with water- and methanol-annealed films the films prepared by slow drying had better mechanical ductility and were more rapidly enzymatically degraded, reflecting the differences in secondary structure achieved via differences in post processing of the cast silk films. Importantly, the silk I structure, a key intermediate secondary structure for the formation of mechanically robust natural silk fibers, was successfully generated by the present approach of very slow drying, mimicking the natural process. The results also point to a new mode of generating new types of silk biomaterials with enhanced mechanical properties and increased degradation rates, while maintaining water insolubility, along with a low beta-sheet content.
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An exothermic transition in SFMA centered at ~224.0 °C is associated with thermally induced structural reorganization and secondary β-sheet formation within the fibroin matrix.
“Importantly, an exothermic transition centered at ~ 224.0 °C was detected and is associated with thermally induced structural reorganization and secondary β-sheet formation within the fibroin matrix, as described by Freddi et al., 1999 andLu et al., 2010 [49,50].”
From Montmorillonite-reinforced methacrylated collagen/methacrylated silk fibroin hydrogel-based inks: rheological and physicochemical characterization for bone scaffold applications (2026) · cites this paper as [50]
Section 3.2 (Thermal stability; page not provided) links a crystallization peak in soluble silk fibroin films at about 213 °C to conversion of non-crystalline structures into β-sheets. This supports the proposed interpretation of a thermal transition, but the paper does not report an SFMA transition centered at about 224 °C. (LLM, conf=0.85)
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- Authors
- Lu, Q., Hu, X., Wang, X., Kluge, J. A., Lu, S., Cebe, P., & Kaplan, D. L.
- Affiliations
- Tufts University (US)
- Corresponding author
- Kaplan, David L.
- Venue
- Acta Biomaterialia
- Publisher
- Elsevier BV
- Published
- 2010-04
- Volume
- 6
- Issue
- 4
- Pages
- 1380-1387
- ISSN
- 1742-7061 (ISSN-L)
- PMC
- PMC2830340
- OpenAlex
- W2017686654
- Cited by
- 654
- References
- 31
- Citations by year
- 2026: 32 · 2025: 32 · 2024: 42 · 2023: 38 · 2022: 46 · 2021: 59 · 2020: 71 · 2019: 49 · 2018: 56 · 2017: 49 · 2016: 36 · 2015: 36 · 2014: 38 · 2013: 17 · 2012: 28
- FWCI
- 7.61
- Type
- journal article
- Language
- en
- Open access
- green
- www.ncbi.nlm.nih.gov
- Locations
- Acta Biomaterialia (publishedVersion)
- PubMed (publishedVersion)
- Europe PMC (PubMed Central) (acceptedVersion)
- PubMed Central (acceptedVersion)
- Funders
- National Science Foundation
- National Institutes of Health
- National Eye Institute (R01EY020856)
- National Institute of Biomedical Imaging and Bioengineering (R01EB003210, P41EB002520)
- National Institute of Dental and Craniofacial Research (R01DE017207)
- Air Force Office of Scientific Research
- Topics
- Physical Sciences › Materials Science › Biomaterials › Silk-based biomaterials and applications
- Life Sciences › Agricultural and Biological Sciences › Insect Science › Silkworms and Sericulture Research
- Physical Sciences › Materials Science › Biomaterials › biodegradable polymer synthesis and properties
- Keywords
- Bombyx mori silk, slow drying, β-sheet content, thermal stability, mechanical properties, enzymatic degradation, silk biomaterials
- MeSH terms
- Calorimetry, Differential Scanning, Pronase, Scattering, Radiation, Solubility, Temperature, Thermogravimetry, Time Factors, Water, X-Ray Diffraction, Protein Structure, Secondary, Spectroscopy, Fourier Transform Infrared, Silk, Mechanical Phenomena
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