Does Supramolecular Gelation Require an External Trigger?

Ruben Van Lommel, Julie Van Hooste, Johannes Vandaele, Gert Steurs, Tom Van der Donck, Frank De Proft, Susana Rocha, Dimitrios Sakellariou, Mercedes Alonso, Wim M. De Borggraeve

Research output: Contribution to journalArticlepeer-review

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.
Original languageEnglish
Article number813
Number of pages13
JournalGels (Basel, Switzerland)
Volume8
Issue number12
DOIs
Publication statusPublished - 10 Dec 2022

Bibliographical note

Funding Information:
R.V.L., G.S. and J.V. thank FWO-Vlaanderen for the PhD fellowships received (1185221N, 1SC3121N, and 1186220N). M.A. thanks the FWO for a postdoctoral fellowship (12F4416N) and the VUB for financial support. F.D.P. and M.A. acknowledge the Vrije Universiteit Brussels for a Strategic Research Program awarded to the ALGC research group. S. R. acknowledges FWO for the research project awarded (G0A5817N). R.V.L. acknowledges the use of Tier2 computational resources and services provided by the Shared ICT Services Center funded by the Vrije Universiteit Brussel, the Flemish Supercomputer Center (VSC), and FWO.

Funding Information:
This research was funded by FWO-Vlaanderen under grant numbers 1185221N (R.V.L.), 1SC3121N (G.S.), 12F4416N (M.A.), 1186220N (J.V.), and G0A5817N (S.R.) and the Strategic Research Program awarded to the ALGC research group by the Vrije Universiteit Brussel (VUB).

Publisher Copyright:
© 2022 by the authors.

Keywords

  • gels
  • self-assembly
  • single particle tracking
  • external stimuli
  • LMWG

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