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Solute addition to solvents causes increased viscosity by structuring the first solvation shell, leading to a jamming transition. This explains viscosity increases in concentrated solutions and challenges traditional models.

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Area of Science:

  • Physical Chemistry
  • Solution Chemistry
  • Rheology

Background:

  • Viscosity increase in concentrated solutions is a long-standing problem.
  • Mayonnaise formation exemplifies a thousand-fold viscosity increase due to structuring.
  • Classical models struggle to explain dramatic viscosity changes.

Purpose of the Study:

  • To explain the dramatic viscosity increase in highly concentrated solutions.
  • To propose a new framework based on solute-induced structuring and jamming transitions.
  • To re-evaluate the utility of the Jones-Dole B-coefficient.

Main Methods:

  • Theoretical analysis of solute-solvent interactions.
  • Modeling of solvation shell structuring.
  • Investigation of jamming transitions in concentrated solutions.

Main Results:

  • Viscosity increase is linked to solute-induced structuring of the first solvation shell.
  • A jamming transition occurs at a critical solute concentration.
  • Viscosity follows a Vogel-Fulcher-Tammann expression as the jamming transition is approached.

Conclusions:

  • Solute-induced structuring and jamming transitions provide a unified explanation for viscosity increase.
  • The Jones-Dole B-coefficient may not accurately reflect structure-making or breaking abilities.
  • This work offers a new perspective on the physical chemistry of concentrated solutions.