Optimization of hybrid gelatin-polysaccharide bioinks exploiting thiol-norbornene chemistry using a reducing additive
- Author
- Nathan Carpentier, Laurens Parmentier (UGent) , Louis Van der Meeren (UGent) , Andre Skirtach (UGent) , Peter Dubruel (UGent) and Sandra Van Vlierberghe (UGent)
- Organization
- Project
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- Capturing the biophysical cues of bone to stimulate bone regeneration in critical bone defects
- Atomic force microscopy (AFM) - nanobiotechnology gebaseerd platform voor het bereiken van de dynamiek van afzonderlijke moleculen tot veelzijdige materialen en celmechanica
- Development of a superior in vitro model for drug hepatoxicity screening through 3D printing of crosslinkable biopolymers.
- Abstract
- Thiol-norbornene chemistry offers great potential in the field of hydrogel development, given its step growth crosslinking mechanism. However, limitations exist with regard to deposition-based bioprinting of thiol-containing hydrogels, associated with premature crosslinking of thiolated (bio)polymers resulting from disulfide formation in the presence of oxygen. More specifically, disulfide formation can result in an increase in viscosity thereby impeding the printing process. In the present work, hydrogels constituting norbornene-modified dextran (DexNB) combined with thiolated gelatin (GelSH) are selected as case study to explore the potential of incorporating the reducing agent tris(2-carboxyethyl)phosphine (TCEP), to prevent the formation of disulfides. We observed that, in addition to preventing disulfide formation, TCEP also contributed to premature, spontaneous thiol-norbornene crosslinking without the use of UV light as evidenced via 1H-NMR spectroscopy. Herein, an optimal concentration of 25 mol% TCEP with respect to the amount of thiols was found, thereby limiting auto-gelation by both minimizing disulfide formation and spontaneous thiol-norbornene reaction. This concentration results in a constant viscosity during at least 24 hours, a more homogeneous network being formed as evidenced using atomic force microscopy while retaining bioink biocompatibility as evidenced by a cell viability of human foreskin fibroblasts exceeding 70 % according to ISO 10993-6:2016.
- Keywords
- Biomedical Engineering, Biomaterials, Bioengineering, viscosity, norbornene-modified biopolymers, bioink, thiolated biopolymers, bioprinting
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Carpentieretal 2024 Biomed. Mater. 10.1088 1748-605X ad2211.pdf
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Citation
Please use this url to cite or link to this publication: http://hdl.handle.net/1854/LU-01HN2Q7TG4K2JF0MPB1DH4TD0H
- MLA
- Carpentier, Nathan, et al. “Optimization of Hybrid Gelatin-Polysaccharide Bioinks Exploiting Thiol-Norbornene Chemistry Using a Reducing Additive.” BIOMEDICAL MATERIALS, vol. 19, no. 2, 2024, doi:10.1088/1748-605x/ad2211.
- APA
- Carpentier, N., Parmentier, L., Van der Meeren, L., Skirtach, A., Dubruel, P., & Van Vlierberghe, S. (2024). Optimization of hybrid gelatin-polysaccharide bioinks exploiting thiol-norbornene chemistry using a reducing additive. BIOMEDICAL MATERIALS, 19(2). https://doi.org/10.1088/1748-605x/ad2211
- Chicago author-date
- Carpentier, Nathan, Laurens Parmentier, Louis Van der Meeren, Andre Skirtach, Peter Dubruel, and Sandra Van Vlierberghe. 2024. “Optimization of Hybrid Gelatin-Polysaccharide Bioinks Exploiting Thiol-Norbornene Chemistry Using a Reducing Additive.” BIOMEDICAL MATERIALS 19 (2). https://doi.org/10.1088/1748-605x/ad2211.
- Chicago author-date (all authors)
- Carpentier, Nathan, Laurens Parmentier, Louis Van der Meeren, Andre Skirtach, Peter Dubruel, and Sandra Van Vlierberghe. 2024. “Optimization of Hybrid Gelatin-Polysaccharide Bioinks Exploiting Thiol-Norbornene Chemistry Using a Reducing Additive.” BIOMEDICAL MATERIALS 19 (2). doi:10.1088/1748-605x/ad2211.
- Vancouver
- 1.Carpentier N, Parmentier L, Van der Meeren L, Skirtach A, Dubruel P, Van Vlierberghe S. Optimization of hybrid gelatin-polysaccharide bioinks exploiting thiol-norbornene chemistry using a reducing additive. BIOMEDICAL MATERIALS. 2024;19(2).
- IEEE
- [1]N. Carpentier, L. Parmentier, L. Van der Meeren, A. Skirtach, P. Dubruel, and S. Van Vlierberghe, “Optimization of hybrid gelatin-polysaccharide bioinks exploiting thiol-norbornene chemistry using a reducing additive,” BIOMEDICAL MATERIALS, vol. 19, no. 2, 2024.
@article{01HN2Q7TG4K2JF0MPB1DH4TD0H,
abstract = {{Thiol-norbornene chemistry offers great potential in the field of hydrogel development, given its step growth crosslinking mechanism. However, limitations exist with regard to deposition-based bioprinting of thiol-containing hydrogels, associated with premature crosslinking of thiolated (bio)polymers resulting from disulfide formation in the presence of oxygen. More specifically, disulfide formation can result in an increase in viscosity thereby impeding the printing process. In the present work, hydrogels constituting norbornene-modified dextran (DexNB) combined with thiolated gelatin (GelSH) are selected as case study to explore the potential of incorporating the reducing agent tris(2-carboxyethyl)phosphine (TCEP), to prevent the formation of disulfides. We observed that, in addition to preventing disulfide formation, TCEP also contributed to premature, spontaneous thiol-norbornene crosslinking without the use of UV light as evidenced via 1H-NMR spectroscopy. Herein, an optimal concentration of 25 mol% TCEP with respect to the amount of thiols was found, thereby limiting auto-gelation by both minimizing disulfide formation and spontaneous thiol-norbornene reaction. This concentration results in a constant viscosity during at least 24 hours, a more homogeneous network being formed as evidenced using atomic force microscopy while retaining bioink biocompatibility as evidenced by a cell viability of human foreskin fibroblasts exceeding 70 % according to ISO 10993-6:2016.}},
articleno = {{025025}},
author = {{Carpentier, Nathan and Parmentier, Laurens and Van der Meeren, Louis and Skirtach, Andre and Dubruel, Peter and Van Vlierberghe, Sandra}},
issn = {{1748-6041}},
journal = {{BIOMEDICAL MATERIALS}},
keywords = {{Biomedical Engineering,Biomaterials,Bioengineering,viscosity,norbornene-modified biopolymers,bioink,thiolated biopolymers,bioprinting}},
language = {{eng}},
number = {{2}},
pages = {{11}},
title = {{Optimization of hybrid gelatin-polysaccharide bioinks exploiting thiol-norbornene chemistry using a reducing additive}},
url = {{http://doi.org/10.1088/1748-605x/ad2211}},
volume = {{19}},
year = {{2024}},
}
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