Catrouillet, Sylvain, Brendel, Johannes C., Larnaudie, Sophie, Barlow, Tammie R., Jolliffe, Katrina A. and Perrier, Sébastien (2016) Tunable length of cyclic peptide–polymer conjugate self-assemblies in water. ACS Macro Letters, 5 (10). pp. 1119-1123. doi:10.1021/acsmacrolett.6b00586 ISSN 2161-1653.

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Abstract

Polymers conjugated to cyclic peptides capable of forming strong hydrogen bonds can self-assemble into supramolecular bottlebrushes even in aqueous solutions. However, controlling the aggregation of these supramolecular assemblies remains an obstacle that is yet to be overcome. By introducing pH-responsive poly(dimethylamino ethyl methacrylate) (pDMAEMA) arms, the repulsive forces were tuned by adjusting the degree of protonation on the polymer arms. Neutron scattering experiments demonstrated that conjugates in an uncharged state will self-assemble into supramolecular bottlebrushes. Reducing the pH in the system led to a decrease in the number of aggregation, which was reversible by addition of base. Potentiometric titration showed a correlation between the number of aggregation and the degree of ionization of the pDMAEMA arms. Hence, a balance between the strength of the hydrogen bonds and the repulsive electrostatic interactions determines the number of aggregation and extent of self-assembly. The presented work demonstrates that conjugate self-association can be controlled by tuning the charge density on the conjugated polymer arms, paving the way for the use of responsive cyclic peptide conjugates in pharmaceutical applications.

Item Type:	Journal Article
Subjects:	Q Science > QD Chemistry
Divisions:	Faculty of Science, Engineering and Medicine > Science > Chemistry
Library of Congress Subject Headings (LCSH):	Peptides, Polymers, Hydrogen bonding
Journal or Publication Title:	ACS Macro Letters
Publisher:	American Chemical Society
ISSN:	2161-1653
Official Date:	19 September 2016
Dates:	Date Event 19 September 2016 Published 12 September 2016 Accepted 1 August 2016 Submitted
Volume:	5
Number:	10
Page Range:	pp. 1119-1123
DOI:	10.1021/acsmacrolett.6b00586
Status:	Peer Reviewed
Publication Status:	Published
Access rights to Published version:	Restricted or Subscription Access
Date of first compliant deposit:	14 November 2016
Date of first compliant Open Access:	19 September 2017
Funder:	Royal Society (Great Britain). Wolfson Research Merit Award (RSWRMA), Monash-Warwick Alliance, Australian Research Council (ARC), Deutsche Forschungsgemeinschaft (DFG), Science and Technology Facilities Council (Great Britain) (STFC)
Grant number:	WM130055 (RSWRMA), DP140100241 (ARC), BR4905/1 (DFG)

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