1. Does Supramolecular Gelation Require an External Trigger?
- Author
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Ruben Van Lommel, Julie Van Hooste, Johannes Vandaele, Gert Steurs, Tom Van der Donck, Frank De Proft, Susana Rocha, Dimitrios Sakellariou, Mercedes Alonso, and Wim M. De Borggraeve
- Subjects
gels ,self-assembly ,single particle tracking ,external stimuli ,LMWG ,Science ,Chemistry ,QD1-999 ,Inorganic chemistry ,QD146-197 ,General. Including alchemy ,QD1-65 - 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.
- Published
- 2022
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