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Self-Assembly of Charge-Containing Copolymers at the Liquid-Liquid Interface.

Felipe Jiménez-Ángeles¹, Ha-Kyung Kwon¹, Kazi Sadman¹

¹Department of Materials Science and Engineering, Department of Chemistry, Department of Chemical and Biological Engineering, and Department of Physics, Northwestern University, Evanston, Illinois 60208, United States.

ACS Central Science

|May 2, 2019

Summary

Amphiphilic block copolymers self-assemble into complex structures at liquid-liquid interfaces, driven by charge interactions. This understanding is key for applications in nanopatterning and drug delivery.

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Area of Science:

Materials Science
Physical Chemistry
Polymer Science

Background:

Understanding amphiphilic macromolecule self-assembly at liquid-liquid interfaces is crucial for applications like drug delivery and nanopatterning.
Complex interactions (hydrophobic, hydrophilic, Coulombic) and environmental factors make studying these phenomena challenging.

Purpose of the Study:

To investigate the self-assembly of a model block copolymer, poly(styrene)-block-poly(2-vinylpyridine) (PS-b-P2VP), and its homopolymer analogue (P2VP) at the chloroform-water interface with varying charge fractions.
To elucidate the driving forces and structural evolution of these self-assembly processes.

Main Methods:

Interfacial tension measurements to quantify polymer adsorption.
Molecular dynamics (MD) simulations to analyze polymer conformation and interfacial aggregate formation.
Controlled quaternization of P2VP to introduce varying, randomly distributed charge fractions.

Main Results:

Polymer adsorption increased significantly with higher charge fractions for the PS-b-P2VP copolymer, while P2VP homopolymers showed greater sensitivity to charged groups.
MD simulations revealed complex interfacial aggregates, including circular domains and elongated stripes, as charge fraction increased.
Observed interfacial structures resembled bulk spherical and cylindrical helicoid structures.

Conclusions:

The self-assembly of charged copolymers at liquid-liquid interfaces is driven by the association of charged components, with hydrophobic segments extending into the non-polar phase.
The study provides quantitative insights into macromolecular self-assembly at interfaces, relevant for designing advanced materials and delivery systems.