Liquid–liquid phase separation during amphiphilic self-assembly

Alessandro Ianiro, Hanglong Wu, Mark M.J. van Rijt, M. Paula Vena, Arthur D.A. Keizer, A. Catarina C. Esteves, Remco Tuinier, Heiner Friedrich, Nico A.J.M. Sommerdijk (Corresponding author), Joseph P. Patterson (Corresponding author)

Research output: Contribution to journalArticleAcademicpeer-review

32 Citations (Scopus)
183 Downloads (Pure)

Abstract

The self-assembly of amphiphilic molecules in solution is a ubiquitous process in both natural and synthetic systems. The ability to effectively control the structure and properties of these systems is essential for tuning the quality of their functionality, yet the underlying mechanisms governing the transition from molecules to assemblies have not been fully resolved. Here we describe how amphiphilic self-assembly can be preceded by liquid–liquid phase separation. The assembly of a model block co-polymer system into vesicular structures was probed through a combination of liquid-phase electron microscopy, self-consistent field computations and Gibbs free energy calculations. This analysis shows the formation of polymer-rich liquid droplets that act as a precursor in the bottom-up formation of spherical micelles, which then evolve into vesicles. The liquid–liquid phase separation plays a role in determining the resulting vesicles’ structural properties, such as their size and membrane thickness, and the onset of kinetic traps during self-assembly.

Original languageEnglish
Pages (from-to)320-328
Number of pages9
JournalNature Chemistry
Volume11
Issue number4
DOIs
Publication statusPublished - 1 Apr 2019

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  • Equipment

    Center for Multiscale Electron Microscopy (CMEM)

    Heiner Friedrich (Manager), Rick Joosten (Operator), Demi de Moor (Operator), Pauline Schmit (Operator), Ingeborg Schreur - Piet (Operator), Anne Spoelstra (Operator) & Nina Romme - van Moll (Other)

    Materials and Interface Chemistry

    Facility/equipment: Research lab

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