Thermally-induced shape-memory behavior of degradable gelatin-based networks
- Shape-memory hydrogels (SMH) are multifunctional, actively-moving polymers of interest in biomedicine. In loosely crosslinked polymer networks, gelatin chains may form triple helices, which can act as temporary net points in SMH, depending on the presence of salts. Here, we show programming and initiation of the shape-memory effect of such networks based on a thermomechanical process compatible with the physiological environment. The SMH were synthesized by reaction of glycidylmethacrylated gelatin with oligo(ethylene glycol) (OEG) alpha,omega-dithiols of varying crosslinker length and amount. Triple helicalization of gelatin chains is shown directly by wide-angle X-ray scattering and indirectly via the mechanical behavior at different temperatures. The ability to form triple helices increased with the molar mass of the crosslinker. Hydrogels had storage moduli of 0.27-23 kPa and Young's moduli of 215-360 kPa at 4 degrees C. The hydrogels were hydrolytically degradable, with full degradation to water-soluble products within one weekShape-memory hydrogels (SMH) are multifunctional, actively-moving polymers of interest in biomedicine. In loosely crosslinked polymer networks, gelatin chains may form triple helices, which can act as temporary net points in SMH, depending on the presence of salts. Here, we show programming and initiation of the shape-memory effect of such networks based on a thermomechanical process compatible with the physiological environment. The SMH were synthesized by reaction of glycidylmethacrylated gelatin with oligo(ethylene glycol) (OEG) alpha,omega-dithiols of varying crosslinker length and amount. Triple helicalization of gelatin chains is shown directly by wide-angle X-ray scattering and indirectly via the mechanical behavior at different temperatures. The ability to form triple helices increased with the molar mass of the crosslinker. Hydrogels had storage moduli of 0.27-23 kPa and Young's moduli of 215-360 kPa at 4 degrees C. The hydrogels were hydrolytically degradable, with full degradation to water-soluble products within one week at 37 degrees C and pH = 7.4. A thermally-induced shape-memory effect is demonstrated in bending as well as in compression tests, in which shape recovery with excellent shape-recovery rates R-r close to 100% were observed. In the future, the material presented here could be applied, e.g., as self-anchoring devices mechanically resembling the extracellular matrix.…
Author details: | Axel T. NeffeORCiDGND, Candy LöwenbergGND, Konstanze K. Julich-GrunerGND, Marc BehlORCiDGND, Andreas LendleinORCiDGND |
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DOI: | https://doi.org/10.3390/ijms22115892 |
ISSN: | 1422-0067 |
ISSN: | 1661-6596 |
Pubmed ID: | https://pubmed.ncbi.nlm.nih.gov/34072689 |
Title of parent work (English): | International journal of molecular sciences |
Publisher: | Molecular Diversity Preservation International |
Place of publishing: | Basel |
Publication type: | Article |
Language: | English |
Date of first publication: | 2021/05/31 |
Publication year: | 2021 |
Release date: | 2024/04/11 |
Tag: | active polymer; biopolymer; degradation; mechanical; properties; shape-memory hydrogel |
Volume: | 22 |
Issue: | 11 |
Article number: | 5892 |
Number of pages: | 15 |
Funding institution: | Helmholtz AssociationHelmholtz Association; German Federal Ministry of Education and Research (BMBF)Federal Ministry of Education & Research (BMBF) [0315696A] |
Organizational units: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie |
DDC classification: | 5 Naturwissenschaften und Mathematik / 54 Chemie / 540 Chemie und zugeordnete Wissenschaften |
5 Naturwissenschaften und Mathematik / 57 Biowissenschaften; Biologie / 570 Biowissenschaften; Biologie | |
Peer review: | Referiert |
Publishing method: | Open Access / Gold Open-Access |
DOAJ gelistet | |
License (German): | CC-BY - Namensnennung 4.0 International |