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. 2022 Mar 7;61(11):e202115232.
doi: 10.1002/anie.202115232. Epub 2022 Jan 27.

Site-Specific Functionalization of Recombinant Spider Silk Janus Fibers

Gregor Lang  1 , Carolin Grill  2 , Thomas Scheibel  2
Affiliations

Site-Specific Functionalization of Recombinant Spider Silk Janus Fibers

Gregor Lang et al. Angew Chem Int Ed Engl. .

Abstract

Biotechnological production is a powerful tool to design materials with customized properties. The aim of this work was to apply designed spider silk proteins to produce Janus fibers with two different functional sides. First, functionalization was established through a cysteine-modified silk protein, ntagCys eADF4(κ16). After fiber spinning, gold nanoparticles (AuNPs) were coupled via thiol-ene click chemistry. Significantly reduced electrical resistivity indicated sufficient loading density of AuNPs on such fiber surfaces. Then, Janus fibers were electrospun in a side-by-side arrangement, with "non-functional" eADF4(C16) on the one and "functional" ntagCys eADF4(κ16) on the other side. Post-treatment was established to render silk fibers insoluble in water. Subsequent AuNP binding was highly selective on the ntagCys eADF4(κ16) side demonstrating the potential of such silk-based systems to realize complex bifunctional structures with spatial resolutions in the nano scale.

Keywords: Biphasic Fibers; Conductive Fibers; Janus Fibers; Silk Functionalization; Spider Silk.

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Figures

Figure 1
Figure 1
SEM images of wet‐spun ntagCyseADF4(κ16) fiber (A) and the respective fiber surface before (B) and after (C) surface modification with AuNPs. Potentiostatic measurements were performed to examine the impact of AuNP coating on the electrical resistivity (D).
Scheme 1
Scheme 1
Schematic illustration of a side‐by‐side electro spinning process to produce Janus fibers of two different spider silk proteins, and subsequent covalent binding of AuNPs on the phase, which is site‐specifically functionalized.
Figure 2
Figure 2
Impact of different post‐treatment agents on the secondary structure of electrospun silk Janus fibers. Data were obtained by quantification of FT‐IR spectra via FSD (n=9). Since both phases of the Janus fiber were made of almost identical proteins, the post‐treatment changes were homogeneous throughout the fibers.
Figure 3
Figure 3
SEM images of electrospun Janus fibers made of eADF4(C16) and ntagCyseADF4(κ16) before (A) and after (B) coupling with gold nanoparticles.
See this image and copyright information in PMC

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