Does Supramolecular Gelation Require an External Trigger?

Author:

Van Lommel RubenORCID,Van Hooste Julie,Vandaele JohannesORCID,Steurs GertORCID,Van der Donck Tom,De Proft Frank,Rocha SusanaORCID,Sakellariou Dimitrios,Alonso MercedesORCID,De Borggraeve Wim M.ORCID

Abstract

The supramolecular gelation of small molecules is typically preceded by an external stimulus to trigger the self-assembly. The need for this trigger stems from the metastable nature of most supramolecular gels and can limit their applicability. Herein, we present a small urea-based molecule that spontaneously forms a stable hydrogel by simple mixing without the addition of an external trigger. Single particle tracking experiments and observations made from scanning electron microscopy indicated that triggerless gelation occurred in a similar fashion as the archetypical heat-triggered gelation. These results could stimulate the search for other supramolecular hydrogels that can be obtained by simple mixing. Furthermore, the mechanism of the heat-triggered supramolecular gelation was elucidated by a combination of molecular dynamics simulations and quantitative NMR experiments. Surprisingly, hydrogelation seemingly occurs via a stepwise self-assembly in which spherical nanoparticles mature into an entangled fibrillary network.

Funder

FWO-Vlaanderen

Publisher

MDPI AG

Subject

Polymers and Plastics,Organic Chemistry,Biomaterials,Bioengineering

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