Sulfobetaine hydrogels with a complex multilength-scale hierarchical structure
- Hydrogels with a hierarchical structure were prepared from a new highly water-soluble crosslinker N,N,N',N'-tetramethyl-N,N'-bis(2-ethylmethacrylate)-propyl-1,3-diammonium dibromide and from the sulfobetaine monomer 2-(N-3-sulfopropyl-N,N-dimethyl ammonium)ethyl methacrylate. The free radical polymerization of the two compounds is rapid and yields near-transparent hydrogels with sizes up to 5 cm in diameter. Rheology shows a clear correlation between the monomer-to-crosslinker ratio and the storage and loss moduli of the hydrogels. Cryo-scanning electron microscopy, low-field nuclear magnetic resonance (NMR) spectroscopy, and small-angle X-ray scattering show that the gels have a hierarchical structure with features spanning the nanometer to the sub-millimeter scale. The NMR study is challenged by the marked inhomogeneity of the gels and the complex chemical structure of the sulfobetaine monomer. NMR spectroscopy shows how these complications can be addressed via a novel fitting approach that considers the mobility gradient along theHydrogels with a hierarchical structure were prepared from a new highly water-soluble crosslinker N,N,N',N'-tetramethyl-N,N'-bis(2-ethylmethacrylate)-propyl-1,3-diammonium dibromide and from the sulfobetaine monomer 2-(N-3-sulfopropyl-N,N-dimethyl ammonium)ethyl methacrylate. The free radical polymerization of the two compounds is rapid and yields near-transparent hydrogels with sizes up to 5 cm in diameter. Rheology shows a clear correlation between the monomer-to-crosslinker ratio and the storage and loss moduli of the hydrogels. Cryo-scanning electron microscopy, low-field nuclear magnetic resonance (NMR) spectroscopy, and small-angle X-ray scattering show that the gels have a hierarchical structure with features spanning the nanometer to the sub-millimeter scale. The NMR study is challenged by the marked inhomogeneity of the gels and the complex chemical structure of the sulfobetaine monomer. NMR spectroscopy shows how these complications can be addressed via a novel fitting approach that considers the mobility gradient along the side chain of methacrylate-based monomers.…
Author details: | Ramona IhlenburgORCiDGND, Tobias MaiGND, Andreas F. ThünemannORCiDGND, Ruth Baerenwald, Kay SaalwächterORCiDGND, Joachim KoetzORCiDGND, Andreas TaubertORCiDGND |
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DOI: | https://doi.org/10.1021/acs.jpcb.0c10601 |
ISSN: | 1520-6106 |
ISSN: | 1520-5207 |
Pubmed ID: | https://pubmed.ncbi.nlm.nih.gov/33769825 |
Title of parent work (English): | The journal of physical chemistry : B, Condensed matter, materials, surfaces, interfaces & biophysical chemistry |
Publisher: | American Chemical Society |
Place of publishing: | Washington |
Publication type: | Article |
Language: | English |
Date of first publication: | 2021/03/26 |
Publication year: | 2021 |
Release date: | 2024/02/21 |
Tag: | Defects; Hydrogels; Nuclear magnetic resonance spectroscopy; Scattering; X-ray scattering |
Volume: | 125 |
Issue: | 13 |
Number of pages: | 11 |
First page: | 3398 |
Last Page: | 3408 |
Funding institution: | University of Potsdam [53170000]; DFGGerman Research Foundation (DFG)European Commission [SA 982/14-1, FOR 2811] |
Organizational units: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie |
DDC classification: | 5 Naturwissenschaften und Mathematik / 53 Physik / 530 Physik |
5 Naturwissenschaften und Mathematik / 54 Chemie / 540 Chemie und zugeordnete Wissenschaften | |
Peer review: | Referiert |