journal article·2025-10-29Open access

Biopolymer Fibers of High Strength and Enhanced Orientation by the Synergy of High/Low Molecular Weight Chitosans in Hybrid Biomaterials Processed by Gel Spinning

Tuan Anh Tran, Ingo Doench, Arnaud Kamdem Tamo, Shaghayegh Jahangir, Sofia Marquez-Bravo, Pamela Molina, Martin Helmstaedter, Aliuska Morales Helguera, Christian Gorzelanny, Anayancy Osorio-Madrazo

Journal of Functional Biomaterials· Volume 16· Issue 11

Abstract

High-performance spun bionanocomposite fibers, composed of high-molecular-weight chitosan (HMW), low-molecular-weight chitosan “oligomers” (LMW), and cellulose nanofibers (CNFs), were successfully fabricated via gel spinning of viscous aqueous chitosan (CHI) based formulations into a NaOH coagulation bath. The X-ray diffraction (XRD) analysis revealed that the incorporation of cellulose nanofibers contributed to enhance crystallinity of chitosan in spun fibers. The spinning process, which comprised sequential acidic solubilization, basic neutralization, stretching, and drying steps, produced chitosan/CNF composite fibers with high crystallinity, further enhanced by the incorporation of low molecular weight chitosan. The cellulose nanofibers seem to promote CHI crystallization, by acting as nucleation sites for the nucleation and growth of chitosan crystals, with those latter of LMW further enhancing crystallization and orientation due to higher mobility of shorter polymer chains. Two-dimensional XRD patterns demonstrated the preferential alignment of both CNFs and chitosan crystals along the fiber axis. Increasing the proportion of short-chain chitosan led to a reduction of the viscosity of collodion, facilitating the spinning of solutions with higher polymer concentrations. The X-ray diffraction (XRD) analysis revealed that the addition of low-molecular-weight chitosan (LMW), with an intermediate molecular weight Mw of ~4.4 × 104 g/mol, produced the most significant improvements in the crystallinity index (CrI) and orientation. This structural enhancement corresponded to superior mechanical properties like Young’s modulus, yield stress σy, and stress-at-break σb of the processed composite fibers. By incorporating that intermediate molecular weight chitosan, a Young’s modulus as high as 20 GPa was achieved for the spun composite fibers, which was twice higher than the modulus of around 10 GPa obtained by adding the lowest molecular weight chitosan of Mw ~ 2.9 × 104 g/mol in the composite, and largely above the modulus of around 5 GPa obtained for fiber just spun with chitosan without incorporation of cellulose nanofibers.
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Research context

OpenAlex topics: Advanced Cellulose Research Studies · Nanocomposite Films for Food Packaging · Natural Fiber Reinforced Composites

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Laboratory of Organ Printing, University of Bayreuth, 95447 Bayreuth, Germany

Laboratory for Bioinspired Materials for Biomedical Engineering BMBT, Department of Microsystems Engineering IMTEK, University of Freiburg, 79110 Freiburg, Germany

Experimental Renal and Cardiovascular Research, Department of Nephropathology, Institute of Pathology and Department of Cardiology, Friedrich Alexander University of Erlangen-Nürnberg (FAU), 91054 Erlangen, Germany

Department of Nephrology, University Hospital Freiburg, University of Freiburg, 79106 Freiburg, Germany

Center of Chemical Bioactives, University of Las Villas, Santa Clara 54838, Cuba

Department of Dermatology and Venerology, University Medical Center Hamburg-Eppendorf, 20246 Hamburg, Germany

Polymer Materials Engineering IMP, CNRS UMR 5223, University Claude Bernard Lyon 1, INSA Lyon, University Jean Monnet, 69622 Villeurbanne, France

Funding

German Research Foundation DFG · Open Access Publishing Fund of the University of Bayreuth

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