Kinetically controlled coassembly of multichromophoric peptide hydrogelators and the impacts on energy transport

Ardoña, H. A. M., Draper, E. R. , Citossi, F., Wallace, M., Serpell, L. C., Adams, D. J. and Tovar, J. 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. (doi: 10.1021/jacs.7b04006) (PMID:28578581)

[img]
Preview
Text
142934.pdf - Published Version
Available under License Creative Commons Attribution.

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 pKa differences, whereas HCl addition leads to a rapid formation of mixed components within a nanostructure. Using 1H 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:Articles
Status:Published
Refereed:Yes
Glasgow Author(s) Enlighten ID:Draper, Emily and Adams, Dave
Authors: Ardoña, H. A. M., Draper, E. R., Citossi, F., Wallace, M., Serpell, L. C., Adams, D. J., and Tovar, J. D.
College/School:College of Science and Engineering > School of Chemistry
Journal Name:Journal of the American Chemical Society
Publisher:American Chemical Society
ISSN:0002-7863
ISSN (Online):1520-5126
Published Online:05 June 2017
Copyright Holders:Copyright © 2017 American Chemical Society
First Published:First published in Journal of the American Chemical Society 139(25): 8685-8692
Publisher Policy:Reproduced under a Creative Commons license

University Staff: Request a correction | Enlighten Editors: Update this record

Project CodeAward NoProject NamePrincipal InvestigatorFunder's NameFunder RefLead Dept
768041Multicomponent Supramolecular HydrogelsDave AdamsEngineering and Physical Sciences Research Council (EPSRC)EP/L021978/2SCHOOL OF CHEMISTRY