Kinetically Controlled Coassembly of Multichromophoric Peptide Hydrogelators and the Impacts on Energy Transport



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.

[img] Text
Ardona et al Proof.pdf - Submitted version

Download (6MB)

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
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: 19 Jan 2023 06:53
DOI: 10.1021/jacs.7b04006
Related URLs:
URI: https://livrepository.liverpool.ac.uk/id/eprint/3009750