"Dumb" pH-Independent and Biocompatible Hydrogels Formed by Copolymers of Long-Chain Alkyl Glycidyl Ethers and Ethylene Oxide
- Publikationstyp:
- Zeitschriftenaufsatz
- Metadaten:
-
- Autoren
- Patrick Verkoyen
- Philip Dreier
- Matthias Bros
- Christian Hils
- Holger Schmalz
- Sebastian Seiffert
- Holger Frey
- Autoren-URL
- https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=fis-test-1&SrcAuth=WosAPI&KeyUT=WOS:000562121800018&DestLinkType=FullRecord&DestApp=WOS_CPL
- DOI
- 10.1021/acs.biomac.0c00576
- eISSN
- 1526-4602
- Externe Identifier
- Clarivate Analytics Document Solution ID: ND7ZO
- PubMed Identifier: 32603096
- ISSN
- 1525-7797
- Ausgabe der Veröffentlichung
- 8
- Zeitschrift
- BIOMACROMOLECULES
- Paginierung
- 3152 - 3162
- Datum der Veröffentlichung
- 2020
- Status
- Published
- Titel
- "Dumb" pH-Independent and Biocompatible Hydrogels Formed by Copolymers of Long-Chain Alkyl Glycidyl Ethers and Ethylene Oxide
- Sub types
- Article
- Ausgabe der Zeitschrift
- 21
Datenquelle: Web of Science (Lite)
- Andere Metadatenquellen:
-
- Autoren
- Patrick Verkoyen
- Philip Dreier
- Matthias Bros
- Christian Hils
- Holger Schmalz
- Sebastian Seiffert
- Holger Frey
- DOI
- 10.1021/acs.biomac.0c00576
- eISSN
- 1526-4602
- ISSN
- 1525-7797
- Ausgabe der Veröffentlichung
- 8
- Zeitschrift
- Biomacromolecules
- Sprache
- en
- Online publication date
- 2020
- Paginierung
- 3152 - 3162
- Datum der Veröffentlichung
- 2020
- Status
- Published
- Herausgeber
- American Chemical Society (ACS)
- Herausgeber URL
- http://dx.doi.org/10.1021/acs.biomac.0c00576
- Datum der Datenerfassung
- 2023
- Titel
- “Dumb” pH-Independent and Biocompatible Hydrogels Formed by Copolymers of Long-Chain Alkyl Glycidyl Ethers and Ethylene Oxide
- Ausgabe der Zeitschrift
- 21
Datenquelle: Crossref
- Abstract
- The formation and rheological properties of hydrogels based on amphiphilic ABA triblock polyether copolymers are described, relying solely on the hydrophobic interaction of long-chain alkyl glycidyl ether (AlkGE)- based A-blocks that are combined with a hydrophilic poly(ethylene glycol) (PEG) midblock. Via anionic ring-opening copolymerization (AROP), ethylene oxide (EO) and long-chain alkyl glycidyl ethers (AlkGEs) were copolymerized, using deprotonated poly(ethylene glycol) (PEG) macroinitiators (<i>M</i><sub>n</sub> of 10, 20 kg mol<sup>-1</sup>). The polymerization afforded amphiphilic ABA triblock copolymers with molar masses in the range of 21-32 kg mol<sup>-1</sup> and dispersities (<i>Đ</i>) of <i>Đ</i> = 1.07-1.17. Kinetic studies revealed random copolymerization of EO and AlkGE, indicating random spacing of the hydrophobic AlkGE units by polar EO units. Following this approach, the hydrophobicity of the apolar blocks of amphiphilic ABA triblock polyethers can be tailored. Detailed rheological measurements confirmed the successful formation of hydrogels at different pH values as a consequence of nonpolar interactions and alkyl chain crystallization. Hydrogel formation was also observed at different ionic strengths (i.e., varied salt concentration), based on the hydrophobic aggregates. This behavior is in contrast to other often-used supramolecular cross-linking strategies, such as Coulomb interactions, complexation, or hydrogen bonding. Micro-differential scanning calorimetry (μ-DSC) measurements of the hydrogels revealed crystalline hydrophobic domains with melting temperatures in the physiological temperature range. In 3-[4,5-dimethylthiazol-2-yl]-2,5-diphenyltetrazoliumbromide (MTT) assays, diblock copolymers possessing structural analogy to the triblock copolymers were studied to assess the general cytotoxicity of amphiphilic polyethers bearing long alkyl chains at the polyether backbone, using splenic immune cells. At intermediate polymer concentrations, no cytotoxic effects were observed. This indicates that long-chain alkyl glycidyl ethers are promising for the introduction of highly hydrophobic as well as crystalline motifs at the polyether backbone in hydrogels for biomedical purposes.
- Addresses
- Department of Chemistry, Johannes Gutenberg University Mainz, Duesbergweg 10-14, 55128 Mainz, Germany.
- Autoren
- Patrick Verkoyen
- Philip Dreier
- Matthias Bros
- Christian Hils
- Holger Schmalz
- Sebastian Seiffert
- Holger Frey
- DOI
- 10.1021/acs.biomac.0c00576
- eISSN
- 1526-4602
- Externe Identifier
- PubMed Identifier: 32603096
- Open access
- false
- ISSN
- 1525-7797
- Ausgabe der Veröffentlichung
- 8
- Zeitschrift
- Biomacromolecules
- Schlüsselwörter
- Polyethylene Glycols
- Epoxy Compounds
- Ethylene Oxide
- Polymers
- Hydrogels
- Kinetics
- Hydrogen-Ion Concentration
- Sprache
- eng
- Medium
- Print-Electronic
- Online publication date
- 2020
- Paginierung
- 3152 - 3162
- Datum der Veröffentlichung
- 2020
- Status
- Published
- Datum der Datenerfassung
- 2020
- Titel
- "Dumb" pH-Independent and Biocompatible Hydrogels Formed by Copolymers of Long-Chain Alkyl Glycidyl Ethers and Ethylene Oxide.
- Sub types
- Journal Article
- Ausgabe der Zeitschrift
- 21
Datenquelle: Europe PubMed Central
- Abstract
- The formation and rheological properties of hydrogels based on amphiphilic ABA triblock polyether copolymers are described, relying solely on the hydrophobic interaction of long-chain alkyl glycidyl ether (AlkGE)- based A-blocks that are combined with a hydrophilic poly(ethylene glycol) (PEG) midblock. Via anionic ring-opening copolymerization (AROP), ethylene oxide (EO) and long-chain alkyl glycidyl ethers (AlkGEs) were copolymerized, using deprotonated poly(ethylene glycol) (PEG) macroinitiators (Mn of 10, 20 kg mol-1). The polymerization afforded amphiphilic ABA triblock copolymers with molar masses in the range of 21-32 kg mol-1 and dispersities (Đ) of Đ = 1.07-1.17. Kinetic studies revealed random copolymerization of EO and AlkGE, indicating random spacing of the hydrophobic AlkGE units by polar EO units. Following this approach, the hydrophobicity of the apolar blocks of amphiphilic ABA triblock polyethers can be tailored. Detailed rheological measurements confirmed the successful formation of hydrogels at different pH values as a consequence of nonpolar interactions and alkyl chain crystallization. Hydrogel formation was also observed at different ionic strengths (i.e., varied salt concentration), based on the hydrophobic aggregates. This behavior is in contrast to other often-used supramolecular cross-linking strategies, such as Coulomb interactions, complexation, or hydrogen bonding. Micro-differential scanning calorimetry (μ-DSC) measurements of the hydrogels revealed crystalline hydrophobic domains with melting temperatures in the physiological temperature range. In 3-[4,5-dimethylthiazol-2-yl]-2,5-diphenyltetrazoliumbromide (MTT) assays, diblock copolymers possessing structural analogy to the triblock copolymers were studied to assess the general cytotoxicity of amphiphilic polyethers bearing long alkyl chains at the polyether backbone, using splenic immune cells. At intermediate polymer concentrations, no cytotoxic effects were observed. This indicates that long-chain alkyl glycidyl ethers are promising for the introduction of highly hydrophobic as well as crystalline motifs at the polyether backbone in hydrogels for biomedical purposes.
- Autoren
- Patrick Verkoyen
- Philip Dreier
- Matthias Bros
- Christian Hils
- Holger Schmalz
- Sebastian Seiffert
- Holger Frey
- Autoren-URL
- https://www.ncbi.nlm.nih.gov/pubmed/32603096
- DOI
- 10.1021/acs.biomac.0c00576
- eISSN
- 1526-4602
- Ausgabe der Veröffentlichung
- 8
- Zeitschrift
- Biomacromolecules
- Schlüsselwörter
- Epoxy Compounds
- Ethylene Oxide
- Hydrogels
- Hydrogen-Ion Concentration
- Kinetics
- Polyethylene Glycols
- Polymers
- Sprache
- eng
- Country
- United States
- Paginierung
- 3152 - 3162
- Datum der Veröffentlichung
- 2020
- Status
- Published
- Datum, an dem der Datensatz öffentlich gemacht wurde
- 2021
- Titel
- "Dumb" pH-Independent and Biocompatible Hydrogels Formed by Copolymers of Long-Chain Alkyl Glycidyl Ethers and Ethylene Oxide.
- Sub types
- Journal Article
- Ausgabe der Zeitschrift
- 21
Datenquelle: PubMed
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