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Unusual Structures of Interpolyelectrolyte Complexes: Vesicles and Perforated Vesicles.

A A Glagoleva1, D E Larin1, V V Vasilevskaya1

  • 1A. N. Nesmeyanov Institute of Organoelement Compounds, Russian Academy of Sciences, Moscow 119991, Russia.

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Summary

Interpolyelectrolyte complexes can self-assemble into hollow spherical particles (vesicles) or perforated vesicles in solution. Differences in polyion-solvent affinity drive the formation of these structures, influenced by electrostatic and hydrophobic interactions.

Keywords:
interpolyelectrolyte complexesself-organizationvesicles

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Area of Science:

  • Polymer Science
  • Materials Science
  • Physical Chemistry

Background:

  • Interpolyelectrolyte complexes (IPECs) are formed by the association of oppositely charged polymers.
  • The morphology of IPECs in solution is influenced by various factors including polymer architecture, charge density, and environmental conditions.
  • Understanding IPEC self-assembly is crucial for developing novel materials with controlled structures.

Purpose of the Study:

  • To investigate the spontaneous formation of hollow spherical particles (vesicles) and perforated vesicles from interpolyelectrolyte complexes in dilute solution.
  • To elucidate the role of polyion-solvent affinity and electrostatic interactions in determining IPEC morphology.
  • To theoretically determine the conditions favoring core-shell and hollow vesicular morphologies.

Main Methods:

  • Computer simulations were employed to model the self-assembly of interpolyelectrolyte complexes.
  • Analytical theory was used to derive conditions for different morphologies.
  • Free energy calculations were performed to determine the stability of core-shell and hollow vesicular structures.
  • An order parameter based on spherical harmonics expansion was introduced to analyze pore distribution in perforated vesicles.

Main Results:

  • IPECs can spontaneously form hollow spherical particles (vesicles) or perforated vesicles depending on the polyion-solvent affinity.
  • When electrostatic interactions are weak, hydrophobic attraction leads to "dense core-loose shell" structures in poor solvent.
  • Strong electrostatic interactions favor layered, hollow, and filled morphologies with segregated macroions.
  • Perforated vesicles represent an intermediate morphology between vesicular and structured solid states.
  • The solvent quality influences the pore distribution in perforated vesicles.

Conclusions:

  • The differential affinity of polyions for the solvent is a key factor in the spontaneous formation of vesicular and perforated vesicular IPEC structures.
  • Both electrostatic and hydrophobic interactions play critical roles in dictating the final morphology of IPECs.
  • Theoretical calculations of free energy successfully predict the formation conditions for core-shell and hollow vesicular morphologies.
  • The study provides a theoretical framework for understanding and controlling the self-assembly of IPECs into complex nanostructures.