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Differential scanning fluorimetry illuminates silk feedstock stability and processability.

C Dicko1, N Kasoju2, N Hawkins3

  • 1Department of Chemistry, Division for Pure and Applied Biochemistry, Lund University, Getigevägen 60, 2241, Lund, Sweden. cedric.dicko@tbiokem.lth.se.

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Summary

Bioengineers can now tailor silk properties by understanding how chemical additives affect silk feedstock stability. Differential scanning fluorimetry (DSF) identified three distinct chemical interaction groups, enabling precise control over silk processing.

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Area of Science:

  • Biomaterials Science
  • Polymer Chemistry
  • Thermodynamics

Background:

  • Designing silk feedstock formulations for controlled spinning remains a significant challenge in bioengineering.
  • Differential scanning fluorimetry (DSF) has emerged as a high-throughput screening technique to link silk feedstock processability with its thermal instability transition temperature (Ti).

Purpose of the Study:

  • To investigate the impact of various chemical additives on silk feedstock stability and processability.
  • To categorize chemical interactions affecting silk feedstock based on their influence on thermal transitions.
  • To develop a thermodynamic framework for analyzing silk feedstock stability and predicting processability.

Main Methods:

  • Utilized differential scanning fluorimetry (DSF) to screen a wide range of chemicals influencing solvent quality for silk.
  • Applied multivariate analysis to categorize chemicals into distinct interaction groups (G1, G2, G3).
  • Performed thermodynamic analysis, including pre- and post-transition fitting, to determine van't Hoff enthalpies (ΔHv) and instability temperatures (Ti).

Main Results:

  • Identified three distinct chemical groupings: G1 (native silk-like), G2 (electrostatic interactions), and G3 (chelating interactions).
  • Quantified significant differences in ΔTi and ΔHv values across the three groups, indicating varied effects on silk stability.
  • Determined that G1 marginally stabilizes native silks (ΔΔG = -0.15 ± 0.04 kcal mol⁻¹), while G2 and G3 destabilize them (ΔΔG = 3.8 ± 0.11 and 3.8 ± 0.3 kcal mol⁻¹, respectively).

Conclusions:

  • Native silk exhibits a complex, possibly non-cooperative, multi-step transition, suggesting an ability to sample substates.
  • Chemical additives can induce direct, cooperative transitions with varying stabilization effects, altering silk's energetic plasticity.
  • The fragile tertiary structure of silk is susceptible to changes in solvent quality, highlighting the importance of feedstock formulation for tailored spinning.