Enzymatic co-crosslinking of star-shaped poly(ethylene glycol) tyramine and hyaluronic acid tyramine conjugates provides elastic biocompatible and biodegradable hydrogels
A combination of the viscoelastic properties of hyaluronic acid (HA) and the elastic properties of star shaped 8-arm poly(ethylene glycol) (8-arm PEG) was used to design in-situ forming hydrogels. Hydrogels were prepared by the enzymatic crosslinking of a partially tyramine modified 8-arm PEG and a...
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KeAi Communications Co., Ltd.
2023-02-01
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| Series: | Bioactive Materials |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S2452199X22002419 |
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| author | Rong Wang Xiaobin Huang Bram Zoetebier Pieter J. Dijkstra Marcel Karperien |
| author_facet | Rong Wang Xiaobin Huang Bram Zoetebier Pieter J. Dijkstra Marcel Karperien |
| author_sort | Rong Wang |
| collection | DOAJ |
| description | A combination of the viscoelastic properties of hyaluronic acid (HA) and the elastic properties of star shaped 8-arm poly(ethylene glycol) (8-arm PEG) was used to design in-situ forming hydrogels. Hydrogels were prepared by the enzymatic crosslinking of a partially tyramine modified 8-arm PEG and a tyramine conjugated HA using horseradish peroxidase in the presence of hydrogen peroxide. Hydrogels of the homopolymer conjugates and mixtures thereof were rapidly formed within seconds under physiological conditions at low polymer and enzyme concentrations. Elastic hydrogels with high gel content (≥95%) and high storage moduli (up to 22.4 kPa) were obtained. An in vitro study in the presence of hyaluronidase (100 U/mL) revealed that with increasing PEG content the degradation time of the hybrid hydrogels increased up to several weeks, whereas hydrogels composed of only hyaluronic acid degraded within 2 weeks. Human mesenchymal stem cells (hMSCs) incorporated in the hybrid hydrogels remained viable as shown by a PrestoBlue and a live-dead assay, confirming the biocompatibility of the constructs. The production of an extracellular matrix by re-differentiation of encapsulated human chondrocytes was followed over a period of 28 days. Gene expression indicated that these highly elastic hydrogels induced an enhanced production of collagen type II. At low PEG-TA/HA-TA ratios a higher expression of SOX 9 and ACAN was observed. These results indicate that by modulating the ratio of PEG/HA, injectable hydrogels can be prepared applicable as scaffolds for tissue regeneration applications. |
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| issn | 2452-199X |
| language | English |
| last_indexed | 2024-04-24T08:41:30Z |
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| series | Bioactive Materials |
| spelling | doaj.art-c4bb833592384200b6177811afe3c91a2024-04-16T15:59:09ZengKeAi Communications Co., Ltd.Bioactive Materials2452-199X2023-02-01205363Enzymatic co-crosslinking of star-shaped poly(ethylene glycol) tyramine and hyaluronic acid tyramine conjugates provides elastic biocompatible and biodegradable hydrogelsRong Wang0Xiaobin Huang1Bram Zoetebier2Pieter J. Dijkstra3Marcel Karperien4Department of Developmental BioEngineering, Faculty of Science and Technology, Tech Med Centre, University of Twente, P.O. Box 217, 7500 AE, Enschede, the NetherlandsDepartment of Developmental BioEngineering, Faculty of Science and Technology, Tech Med Centre, University of Twente, P.O. Box 217, 7500 AE, Enschede, the NetherlandsDepartment of Developmental BioEngineering, Faculty of Science and Technology, Tech Med Centre, University of Twente, P.O. Box 217, 7500 AE, Enschede, the NetherlandsDepartment of Developmental BioEngineering, Faculty of Science and Technology, Tech Med Centre, University of Twente, P.O. Box 217, 7500 AE, Enschede, the NetherlandsCorresponding author.; Department of Developmental BioEngineering, Faculty of Science and Technology, Tech Med Centre, University of Twente, P.O. Box 217, 7500 AE, Enschede, the NetherlandsA combination of the viscoelastic properties of hyaluronic acid (HA) and the elastic properties of star shaped 8-arm poly(ethylene glycol) (8-arm PEG) was used to design in-situ forming hydrogels. Hydrogels were prepared by the enzymatic crosslinking of a partially tyramine modified 8-arm PEG and a tyramine conjugated HA using horseradish peroxidase in the presence of hydrogen peroxide. Hydrogels of the homopolymer conjugates and mixtures thereof were rapidly formed within seconds under physiological conditions at low polymer and enzyme concentrations. Elastic hydrogels with high gel content (≥95%) and high storage moduli (up to 22.4 kPa) were obtained. An in vitro study in the presence of hyaluronidase (100 U/mL) revealed that with increasing PEG content the degradation time of the hybrid hydrogels increased up to several weeks, whereas hydrogels composed of only hyaluronic acid degraded within 2 weeks. Human mesenchymal stem cells (hMSCs) incorporated in the hybrid hydrogels remained viable as shown by a PrestoBlue and a live-dead assay, confirming the biocompatibility of the constructs. The production of an extracellular matrix by re-differentiation of encapsulated human chondrocytes was followed over a period of 28 days. Gene expression indicated that these highly elastic hydrogels induced an enhanced production of collagen type II. At low PEG-TA/HA-TA ratios a higher expression of SOX 9 and ACAN was observed. These results indicate that by modulating the ratio of PEG/HA, injectable hydrogels can be prepared applicable as scaffolds for tissue regeneration applications.http://www.sciencedirect.com/science/article/pii/S2452199X22002419PEG-OH8HAEnzymatic crosslinking hydrogelDegradationProliferation & differentiation |
| spellingShingle | Rong Wang Xiaobin Huang Bram Zoetebier Pieter J. Dijkstra Marcel Karperien Enzymatic co-crosslinking of star-shaped poly(ethylene glycol) tyramine and hyaluronic acid tyramine conjugates provides elastic biocompatible and biodegradable hydrogels Bioactive Materials PEG-OH8 HA Enzymatic crosslinking hydrogel Degradation Proliferation & differentiation |
| title | Enzymatic co-crosslinking of star-shaped poly(ethylene glycol) tyramine and hyaluronic acid tyramine conjugates provides elastic biocompatible and biodegradable hydrogels |
| title_full | Enzymatic co-crosslinking of star-shaped poly(ethylene glycol) tyramine and hyaluronic acid tyramine conjugates provides elastic biocompatible and biodegradable hydrogels |
| title_fullStr | Enzymatic co-crosslinking of star-shaped poly(ethylene glycol) tyramine and hyaluronic acid tyramine conjugates provides elastic biocompatible and biodegradable hydrogels |
| title_full_unstemmed | Enzymatic co-crosslinking of star-shaped poly(ethylene glycol) tyramine and hyaluronic acid tyramine conjugates provides elastic biocompatible and biodegradable hydrogels |
| title_short | Enzymatic co-crosslinking of star-shaped poly(ethylene glycol) tyramine and hyaluronic acid tyramine conjugates provides elastic biocompatible and biodegradable hydrogels |
| title_sort | enzymatic co crosslinking of star shaped poly ethylene glycol tyramine and hyaluronic acid tyramine conjugates provides elastic biocompatible and biodegradable hydrogels |
| topic | PEG-OH8 HA Enzymatic crosslinking hydrogel Degradation Proliferation & differentiation |
| url | http://www.sciencedirect.com/science/article/pii/S2452199X22002419 |
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