Ardona, Herdeline Ann M, Draper, Emily R, Citossi, Francesca, Wallace, Matthew, Serpell, Louise C, Adams, Dave J and Tovar, John D
(2017)
Kinetically Controlled Coassembly of Multichromophoric Peptide Hydrogelators and the Impacts on Energy Transport.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 139 (25).
pp. 8685-8692.
ISSN 0002-7863, 1520-5126
Text
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Abstract
We report a peptide-based multichromophoric hydrogelator system, wherein π-electron units with different inherent spectral energies are spatially controlled within peptidic 1-D nanostructures to create localized energy gradients in aqueous environments. This is accomplished by mixing different π-conjugated peptides prior to initiating self-assembly through solution acidification. We can vary the kinetics of the assembly and the degree of self-sorting through the choice of the assembly trigger, which changes the kinetics of acidification. The hydrolysis of glucono-δ-lactone (GdL) provides a slow pH drop that allows for stepwise triggering of peptide components into essentially self-sorted nanostructures based on subtle pK<sub>a</sub> differences, whereas HCl addition leads to a rapid formation of mixed components within a nanostructure. Using <sup>1</sup>H NMR spectroscopy and fiber X-ray diffraction, we determine the conditions and peptide mixtures that favor self-sorting or intimate comixing. Photophysical investigations in the solution phase provide insight into the correlation of energy-transport processes occurring within the assemblies to the structural organization of the π-systems.
Item Type: | Article |
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Uncontrolled Keywords: | Peptides, Hydrogels, Microscopy, Electron, Transmission, X-Ray Diffraction, Magnetic Resonance Spectroscopy, Molecular Structure, Kinetics, Nanostructures |
Depositing User: | Symplectic Admin |
Date Deposited: | 04 Oct 2017 06:31 |
Last Modified: | 07 Dec 2024 18:41 |
DOI: | 10.1021/jacs.7b04006 |
Related URLs: | |
URI: | https://livrepository.liverpool.ac.uk/id/eprint/3009750 |