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G4-Quartet·M+Borate Hydrogels
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Peters, Gretchen Marie, Skala, Luke P., Plank, Taylor N., Oh, Hyuntaek, Reddy, G. N. Manjunatha, Marsh, Andrew, Brown, Steven P., Raghavan, Srinivasa R. and Davis, Jeffery T. (2015) G4-Quartet·M+Borate Hydrogels. Journal of the American Chemical Society, 137 (17). pp. 5819-5827. doi:10.1021/jacs.5b02753
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Official URL: http://dx.doi.org/10.1021/jacs.5b02753
Abstract
The ability to modulate the physical properties of a supramolecular hydrogel may be beneficial for biomaterial and biomedical applications. We find that guanosine (G 1), when combined with 0.5 equiv of potassium borate, forms a strong, self-supporting hydrogel with elastic moduli >10 kPa. The countercation in the borate salt (MB(OH)4) significantly alters the physical properties of the hydrogel. The gelator combination of G 1 and KB(OH)4 formed the strongest hydrogel, while the weakest system was obtained with LiB(OH)4, as judged by 1H NMR and rheology. Data from powder XRD, 1H double-quantum solid-state magic-angle spinning (MAS) NMR and small-angle neutron scattering (SANS) were consistent with a structural model that involves formation of borate dimers and G4·K+ quartets by G 1 and KB(OH)4. Stacking of these G4·M+ quartets into G4-nanowires gives a hydrogel. We found that the M+ cation helps stabilize the anionic guanosine-borate (GB) diesters, as well as the G4-quartets. Supplementing the standard gelator mixture of G 1 and 0.5 equiv of KB(OH)4 with additional KCl or KNO3 increased the strength of the hydrogel. We found that thioflavin T fluoresces in the presence of G4·M+ precursor structures. This fluorescence response for thioflavin T was the greatest for the K+ GB system, presumably due to the enhanced interaction of the dye with the more stable G4·K+ quartets. The fluorescence of thioflavin T increased as a function of gelator concentration with an increase that correlated with the system’s gel point, as measured by solution viscosity
| Item Type: | Journal Article | ||||||
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| Subjects: | Q Science > QD Chemistry | ||||||
| Divisions: | Faculty of Science > Chemistry Faculty of Science > Physics |
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| Library of Congress Subject Headings (LCSH): | Colloids | ||||||
| Journal or Publication Title: | Journal of the American Chemical Society | ||||||
| Publisher: | American Chemical Society | ||||||
| ISSN: | 0002-7863 | ||||||
| Official Date: | 14 April 2015 | ||||||
| Dates: |
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| Volume: | 137 | ||||||
| Number: | 17 | ||||||
| Number of Pages: | 8 | ||||||
| Page Range: | pp. 5819-5827 | ||||||
| DOI: | 10.1021/jacs.5b02753 | ||||||
| Status: | Peer Reviewed | ||||||
| Publication Status: | Published | ||||||
| Access rights to Published version: | Open Access | ||||||
| Funder: | United States. Department of Energy, Engineering and Physical Sciences Research Council (EPSRC) | ||||||
| Grant number: | DE-FG01- 98ER14888 (DOE), EP/K003674/1 (EPSRC) |
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