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Single core and multicore aggregates from a polymer mixture: A dissipative particle dynamics study.

Sousa Javan Nikkhah1, Maria Sammalkorpi2

  • 1Department of Chemistry and Materials Science, School of Chemical Engineering, Aalto University, P.O. Box 16100, FI-00076 Aalto, Finland; Department of Physics, Bernal Institute, University of Limerick, V94 T9PX Limerick, Ireland; Department of Chemical Sciences, Bernal Institute, University of Limerick, V94 T9PX Limerick, Ireland.

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|January 1, 2023
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Summary

The concentration of block copolymer controls self-assembly into multicore or single-core polymer aggregates. A minimum solvent incompatibility is also required for multicore formation, guiding the design of novel polymer capsules.

Keywords:
Coarse-grained simulationsDissipative particle dynamicsMulticore aggregatePolymeric aggregateSingle core-double shell aggregateStructural transition

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Area of Science:

  • Polymer Science
  • Materials Chemistry
  • Computational Chemistry

Background:

  • Multicore block copolymer aggregates are self-assembled structures with multiple, distinct droplet-like cores.
  • These aggregates serve as versatile capsules for applications like drug delivery, catalysis, and chemical reactions.
  • Polymer system composition is hypothesized to control self-assembly into these useful morphologies.

Purpose of the Study:

  • To investigate the self-assembly of polymer mixtures into multicore or single-core aggregates.
  • To determine the influence of block copolymer concentration, component ratios, and homopolymer chain length on aggregate structure.
  • To establish guidelines for designing polymer systems that yield specific aggregate morphologies.

Main Methods:

  • Dissipative particle dynamics (DPD) simulations were employed to model the self-assembly process.
  • The study examined mixtures of highly and weakly solvophobic homopolymers with an amphiphilic block copolymer in a solvent.
  • Assembly response (multicore vs. single-core) was mapped against varying parameters.

Main Results:

  • Block copolymer concentration is the primary factor determining single-core versus multicore aggregation.
  • A critical copolymer concentration exists for multicore aggregation, dependent on the specific polymer system.
  • Sufficient incompatibility between the solvent and the weakly solvophobic component is necessary for multicore assembly.

Conclusions:

  • The study provides critical insights into controlling polymer self-assembly for targeted aggregate formation.
  • Guidelines are presented for tuning assembly between multicore and single-core (core-shell) structures.
  • This research facilitates the rational design of polymer systems for advanced capsule applications.