Supramolecular polymers form tactoids through liquid–liquid phase separation

Hailin Fu (), Jingyi Huang, Joost J. B. van der Tol, Lu Su, Yuyang Wang, Swayandipta Dey, Peter Zijlstra, George Fytas, Ghislaine Vantomme, Patricia Y. W. Dankers and E. W. Meijer ()
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Hailin Fu: Eindhoven University of Technology
Jingyi Huang: Eindhoven University of Technology
Joost J. B. van der Tol: Eindhoven University of Technology
Lu Su: Leiden University
Yuyang Wang: Eindhoven University of Technology
Swayandipta Dey: Eindhoven University of Technology
Peter Zijlstra: Eindhoven University of Technology
George Fytas: Eindhoven University of Technology
Ghislaine Vantomme: Eindhoven University of Technology
Patricia Y. W. Dankers: Eindhoven University of Technology
E. W. Meijer: Eindhoven University of Technology

Nature, 2024, vol. 626, issue 8001, 1011-1018

Abstract: Abstract Liquid–liquid phase separation (LLPS) of biopolymers has recently been shown to play a central role in the formation of membraneless organelles with a multitude of biological functions1–3. The interplay between LLPS and macromolecular condensation is part of continuing studies4,5. Synthetic supramolecular polymers are the non-covalent equivalent of macromolecules but they are not reported to undergo LLPS yet. Here we show that continuously growing fibrils, obtained from supramolecular polymerizations of synthetic components, are responsible for phase separation into highly anisotropic aqueous liquid droplets (tactoids) by means of an entropy-driven pathway. The crowding environment, regulated by dextran concentration, affects not only the kinetics of supramolecular polymerizations but also the properties of LLPS, including phase-separation kinetics, morphology, internal order, fluidity and mechanical properties of the final tactoids. In addition, substrate–liquid and liquid–liquid interfaces proved capable of accelerating LLPS of supramolecular polymers, allowing the generation of a myriad of three-dimensional-ordered structures, including highly ordered arrays of micrometre-long tactoids at surfaces. The generality and many possibilities of supramolecular polymerizations to control emerging morphologies are demonstrated with several supramolecular polymers, opening up a new field of matter ranging from highly structured aqueous solutions by means of stabilized LLPS to nanoscopic soft matter.

Date: 2024
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DOI: 10.1038/s41586-024-07034-7

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