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Volume 13
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10.3390/polym13101663
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Article

Development of Bioinspired Functional Chitosan/Cellulose Nanofiber 3D Hydrogel Constructs by 3D Printing for Application in the Engineering of Mechanically Demanding Tissues

by
Arnaud Kamdem Tamo
1,2,3,
Ingo Doench
1,2,3,
Lukas Walter
1,2,3,
Alexandra Montembault
4,
Guillaume Sudre
4,
Laurent David
4,
Aliuska Morales-Helguera
5,
Mischa Selig
6,
Bernd Rolauffs
6,
Anke Bernstein
6,
Daniel Hoenders
7,
Andreas Walther
7 and
Anayancy Osorio-Madrazo
1,2,3,*
1
Laboratory for Sensors, Institute of Microsystems Engineering IMTEK, University of Freiburg, 79110 Freiburg, Germany
2
Freiburg Materials Research Center—FMF, University of Freiburg, 79104 Freiburg, Germany
3
Freiburg Center for Interactive Materials and Bioinspired Technologies—FIT, University of Freiburg, 79110 Freiburg, Germany
4
Ingénierie des Matériaux Polymères IMP UMR 5223—CNRS, Université Claude Bernard Lyon 1, Université de Lyon, CEDEX, 69622 Villeurbanne, France
5
Chemical Bioactive Center CBQ, Molecular Simulation and Drug Design Group, Central University of Las Villas, Santa Clara 50400, Cuba
6
Center for Tissue Replacement, Regeneration & Neogenesis—G.E.R.N., Department of Orthopedics and Trauma Surgery, University of Freiburg, 79108 Freiburg, Germany
7
Department of Chemistry, University Mainz, 55128 Mainz, Germany
*
Author to whom correspondence should be addressed.
Polymers 2021, 13(10), 1663; https://doi.org/10.3390/polym13101663
Submission received: 1 May 2021 / Revised: 14 May 2021 / Accepted: 17 May 2021 / Published: 20 May 2021
(This article belongs to the Special Issue Chitosan, Chitin, and Cellulose Nanofiber Biomaterials)
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Abstract

Soft tissues are commonly fiber-reinforced hydrogel composite structures, distinguishable from hard tissues by their low mineral and high water content. In this work, we proposed the development of 3D printed hydrogel constructs of the biopolymers chitosan (CHI) and cellulose nanofibers (CNFs), both without any chemical modification, which processing did not incorporate any chemical crosslinking. The unique mechanical properties of native cellulose nanofibers offer new strategies for the design of environmentally friendly high mechanical performance composites. In the here proposed 3D printed bioinspired CNF-filled CHI hydrogel biomaterials, the chitosan serves as a biocompatible matrix promoting cell growth with balanced hydrophilic properties, while the CNFs provide mechanical reinforcement to the CHI-based hydrogel. By means of extrusion-based printing (EBB), the design and development of 3D functional hydrogel scaffolds was achieved by using low concentrations of chitosan (2.0–3.0% (w/v)) and cellulose nanofibers (0.2–0.4% (w/v)). CHI/CNF printed hydrogels with good mechanical performance (Young’s modulus 3.0 MPa, stress at break 1.5 MPa, and strain at break 75%), anisotropic microstructure and suitable biological response, were achieved. The CHI/CNF composition and processing parameters were optimized in terms of 3D printability, resolution, and quality of the constructs (microstructure and mechanical properties), resulting in good cell viability. This work allows expanding the library of the so far used biopolymer compositions for 3D printing of mechanically performant hydrogel constructs, purely based in the natural polymers chitosan and cellulose, offering new perspectives in the engineering of mechanically demanding hydrogel tissues like intervertebral disc (IVD), cartilage, meniscus, among others.
Keywords: hydrogel 3D printing; polymer composites; chitosan; cellulose nanofibers; X-ray synchrotron scattering; micromechanics; tissue engineering hydrogel 3D printing; polymer composites; chitosan; cellulose nanofibers; X-ray synchrotron scattering; micromechanics; tissue engineering
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MDPI and ACS Style

Kamdem Tamo, A.; Doench, I.; Walter, L.; Montembault, A.; Sudre, G.; David, L.; Morales-Helguera, A.; Selig, M.; Rolauffs, B.; Bernstein, A.; et al. Development of Bioinspired Functional Chitosan/Cellulose Nanofiber 3D Hydrogel Constructs by 3D Printing for Application in the Engineering of Mechanically Demanding Tissues. Polymers 2021, 13, 1663. https://doi.org/10.3390/polym13101663

AMA Style

Kamdem Tamo A, Doench I, Walter L, Montembault A, Sudre G, David L, Morales-Helguera A, Selig M, Rolauffs B, Bernstein A, et al. Development of Bioinspired Functional Chitosan/Cellulose Nanofiber 3D Hydrogel Constructs by 3D Printing for Application in the Engineering of Mechanically Demanding Tissues. Polymers. 2021; 13(10):1663. https://doi.org/10.3390/polym13101663

Chicago/Turabian Style

Kamdem Tamo, Arnaud, Ingo Doench, Lukas Walter, Alexandra Montembault, Guillaume Sudre, Laurent David, Aliuska Morales-Helguera, Mischa Selig, Bernd Rolauffs, Anke Bernstein, and et al. 2021. "Development of Bioinspired Functional Chitosan/Cellulose Nanofiber 3D Hydrogel Constructs by 3D Printing for Application in the Engineering of Mechanically Demanding Tissues" Polymers 13, no. 10: 1663. https://doi.org/10.3390/polym13101663

APA Style

Kamdem Tamo, A., Doench, I., Walter, L., Montembault, A., Sudre, G., David, L., Morales-Helguera, A., Selig, M., Rolauffs, B., Bernstein, A., Hoenders, D., Walther, A., & Osorio-Madrazo, A. (2021). Development of Bioinspired Functional Chitosan/Cellulose Nanofiber 3D Hydrogel Constructs by 3D Printing for Application in the Engineering of Mechanically Demanding Tissues. Polymers, 13(10), 1663. https://doi.org/10.3390/polym13101663

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