Recognition-mediated hydrogel swelling controlled by interaction with a negative thermoresponsive LCST polymer

Belal, K. et al. (2016) Recognition-mediated hydrogel swelling controlled by interaction with a negative thermoresponsive LCST polymer. Angewandte Chemie (International Edition), 55(45), pp. 13974-13978. (doi: 10.1002/anie.201605630) (PMID:27730718)

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Most polymeric thermoresponsive hydrogels contract upon heating beyond the lower critical solution temperature (LCST) of the polymers used. Herein, we report a supramolecular hydrogel system that shows the opposite temperature dependence. When the non-thermosesponsive hydrogel NaphtGel, containing dialkoxynaphthalene guest molecules, becomes complexed with the tetra cationic macrocyclic host CBPQT4+, swelling occurred as a result of host–guest complex formation leading to charge repulsion between the host units, as well as an osmotic contribution of chloride counter-ions embedded in the network. The immersion of NaphtGel in a solution of poly(N-isopropylacrylamide) with tetrathiafulvalene (TTF) end groups complexed with CBPQT4+ induced positive thermoresponsive behaviour. The LCST-induced dethreading of the polymer-based pseudorotaxane upon heating led to transfer of the CBPQT4+ host and a concomitant swelling of NaphtGel. Subsequent cooling led to reformation of the TTF-based host–guest complexes in solution and contraction of the hydrogel.

Item Type:Articles
Glasgow Author(s) Enlighten ID:Cooke, Professor Graeme
Authors: Belal, K., Stoffelbach, F., Lyskawa, J., Fumagalli, M., Hourdet, D., Marcellan, A., De Smet, L., de la Rosa, V. R., Cooke, G., Hoogenboom, R., and Woisel, P.
College/School:College of Science and Engineering > School of Chemistry
Journal Name:Angewandte Chemie (International Edition)
ISSN (Online):1521-3773
Published Online:12 October 2016
Copyright Holders:Copyright © 2016 The Authors
First Published:First published in Angewandte Chemie (International Edition) 55(45): 13974-13978
Publisher Policy:Reproduced under a Creative Commons License

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Project CodeAward NoProject NamePrincipal InvestigatorFunder's NameFunder RefLead Dept
445041Physical organic chemistry - opportunities in synthesis, materials and pharmaceuticalsGraeme CookeEngineering & Physical Sciences Research Council (EPSRC)EP/E036244/1CHEM - CHEMISTRY