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Whether solid, liquid, or gas, a substance's state depends on the order and arrangement of its particles (atoms, molecules, or ions). Particles in the solid pack closely together, generally in a pattern. The particles vibrate about their fixed positions but do not move or squeeze past their neighbors. In liquids, although the particles are closely spaced, they are randomly arranged. The position of the particles are not fixed—that is, they are free to move past their neighbors to...
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The process of surrounding a solute with solvent is called solvation. It involves evenly distributing the solute within the solvent. The rule of thumb for determining a solvent for a given compound is that like dissolves like. A good solvent has molecular characteristics similar to those of the compound to be dissolved. For example, polar solutions dissolve polar solutes, and apolar solvents dissolve apolar solutes. A polar solvent is a solvent that has a high dielectric constant (ϵ...
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Entropy-Driven Liquid-Liquid Phase Separation Transition to Polymeric Micelles.

Morteza Rasoulianboroujeni1, Melgardt M de Villiers1, Glen S Kwon1

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Entropy-driven liquid-liquid phase separation (LLPS) using oligomers as solvents offers a tunable precursor for polymeric micelle formation. This reversible process allows for control over self-assembly in amphiphilic systems.

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Area of Science:

  • Materials Science
  • Physical Chemistry
  • Polymer Science

Background:

  • Liquid-liquid phase separation (LLPS) is increasingly recognized as a precursor to self-assembly in amphiphilic systems.
  • Controlling LLPS is key to understanding and directing self-assembly processes.

Purpose of the Study:

  • To propose and model the use of entropy-driven LLPS as a tunable precursor for polymeric micelle formation.
  • To investigate the influence of solvent oligomerization on LLPS and micellization behavior.

Main Methods:

  • Development of a comprehensive model using mean-field lattice theory.
  • Prediction of LLPS and micellization conditions.
  • Experimental validation using dynamic light scattering and phase microscopy.

Main Results:

  • Solvent degree of polymerization significantly impacts phase behavior, overriding enthalpic contributions.
  • Model predicts LLPS prior to micellization for specific block copolymers (e.g., PEG4kDa-b-PLA2.2kDa) with solvents of degree of polymerization ≥ 5.
  • Experimental results confirm model predictions for PEG4kDa-b-PLA2.2kDa/PEG200/water mixtures, showing LLPS and micellization at specific water content.

Conclusions:

  • Entropy-driven LLPS provides a tunable pathway to polymeric micelle formation.
  • The LLPS-to-micelle transition is reversible, suggesting thermodynamic equilibrium between the phase-separated liquid and micelles.
  • Oligomer solvents offer a novel approach to control self-assembly in block copolymer systems.