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In recent years, food polymer-based Electrospun Nanofbers have attracted significant attention due to the economic and environmental benefits of renewable food resources, and related research has focused extensively on their biopolymer applications. This creates an opportunity for fish food processing wastes (e.g., fish skin, fish scales, and fish bones), which provide a rich source of the natural polymer collagen type I (COL), a natural polymer with a stabilized triple-helical structure consisting of a right-handed, triple-helicoidal structure with three α-subunits. COL has been extensively studied in the biomedical, pharmaceutical, food, and cosmetic industries due to its non-immunogenicity, good biocompatibility, and biodegradability.Type I COL is a major structural protein in the extracellular matrix (ECM) of organs and tissues, and plays a key role in maintaining the biological and structural integrity of the ECM, which is continually being remodeled to achieve physiological functions. Therefore, COL-based materials are currently favored in biomaterials and food packaging manufacturing.
The main point of this paper
Application of electrospinning technology in tissue engineering:
Electrospinning is used to prepare nanofiber scaffolds similar to natural extracellular matrix (ECM).
Challenges of collagen (COL) electrospinning:
For electrospinning, COL needs to be denatured in order to dissolve into an electrospinnable solution, which may lead to the destruction of its structure.
Use of organic solvents and their problems:
The conventional use of highly volatile organic solvents (e.g., HFP and TFE) can lead to denaturation and structural damage of COL.
These solvents are corrosive and toxic and may affect subsequent applications.
Eco-friendly solvent selection:
Acetic acid, as an environmentally friendly and non-toxic solvent, is encouraged to be used as a green solvent by the European Union.
Acetic acid has a positive impact on the preparation of nanofibers and is available from biomass.
Application of Pullulan (PUL):
PUL acts as a GRAS-listed polysaccharide that forms hydrogen bonds with proteins and improves their spinnability.
Research Methods:
Fish COL/PUL ultrafine fibers were prepared by electrospinning using acetic acid as a solvent
Hydrogen bonding interactions between COL and PUL and their effects on COL spinnability were investigated
Prospects for collagen electrospun fibers:
Collagen electrospun fibers have potential in food packaging and tissue engineering
Limitations of conventional preparation methods:
Conventional collagen electrospinning usually uses toxic organic reagents with safety and toxic solvent residue issues
Use of eco-friendly solvents:
In this study, acetic acid was used as the solvent, which is safe and does not produce toxic solvent residues.
Introduction of Pullulan (PUL):
The introduction of PUL increases the degree of entanglement of molecules in solution and improves the spinnability of COL
Change in solution properties:
The viscosity and conductivity of the COL/PUL electrospinning solution changed, with an increase in viscosity and a decrease in conductivity
Morphology and diameter of electrospun fibers:
Smooth and defect-free COL/PUL ultrafine fibers with diameters of 215.32 ± 40.56 nm and 240.97 ± 53.93 nm, respectively, were successfully prepared by scanning electron microscopy analysis
Changes in hydrogen bonding interactions:
As the proportion of PUL increased, intramolecular hydrogen bonding became the main interaction between COL and PUL, and the content of intermolecular hydrogen bonding decreased and intramolecular hydrogen bonding increased
In this study, COL/PUL microfibers were successfully prepared by electrospinning using 0.4 M acetic acid as solvent, and the introduction of PUL helped to increase the intermolecular entanglement of COL and PUL, which improved the spinnability of COL and transformed the morphology of the microfibers from spindle-like to smooth. With the improvement of COL electrospinning solution spinnability, the protein part unfolded and the triple helix part retained more than 36%. FTIR analysis showed that the COL/PUL microfibers tended to form intramolecular hydrogen bonds through the breaking of intermolecular hydrogen bonds after the addition of PUL. In addition, secondary structure analysis showed that the COL gradually unfolded, and the α-helix and β-turn structures were gradually transformed into β-sheet and random coil structures.
In addition, the tensile strength and elongation at break of ultrafine fibers were related to diameter and morphology. Smooth, defect-free, and small-diameter microfibers have excellent mechanical strength and elongation at break. In conclusion, this study successfully prepared COL/PUL microfibers without the use of toxic solvents and investigated the interactions between COL and PUL molecules for improved spinnability, providing useful information for the development of COL-based food fibers.
