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

9 Citations (Scopus)

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.

LanguageEnglish
Pages320-328
Number of pages9
JournalNature Chemistry
Volume11
DOIs
StatePublished - 18 Feb 2019

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Phase separation
Self assembly
Liquids
Polymers
Molecules
Micelles
Gibbs free energy
Electron microscopy
Structural properties
Tuning
Membranes
Kinetics

Cite this

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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.",
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Liquid–liquid phase separation during amphiphilic self-assembly. / Ianiro, Alessandro; Wu, Hanglong; van Rijt, Mark M.J.; Vena, M. Paula; Keizer, Arthur D.A.; Esteves, A. Catarina C.; Tuinier, Remco; Friedrich, Heiner; Sommerdijk, Nico A.J.M. (Corresponding author); Patterson, Joseph P. (Corresponding author).

In: Nature Chemistry, Vol. 11, 18.02.2019, p. 320-328.

Research output: Contribution to journalArticleAcademicpeer-review

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AU - Patterson,Joseph P.

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