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1-propanol/water mixtures exhibit structural and dynamic heterogeneity, forming a phase diagram with liquid phases, ice, and hydrates. Confinement influences water crystallization, revealing insights into ultra-viscous water phases.

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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Thermodynamics

Background:

  • 1-propanol/water mixtures display complex structural and dynamic behaviors.
  • Understanding the phase diagram and molecular interactions is crucial for various applications.

Purpose of the Study:

  • To construct the phase diagram of 1-propanol/water mixtures across the entire composition range.
  • To investigate the structural and dynamic heterogeneity of these mixtures.
  • To explore the influence of confinement on water crystallization and dynamics.

Main Methods:

  • X-ray diffraction for structural analysis.
  • Differential scanning calorimetry for thermodynamic profiling.
  • Dielectric spectroscopy for probing molecular dynamics.

Main Results:

  • A phase diagram comprising liquid 1-propanol, liquid water, hexagonal ice, and various hydrates was established.
  • Four distinct regimes were identified, characterized by droplet arrangements of the minority component.
  • Soft confinement of water by 1-propanol prevented crystallization, yielding dynamics akin to high-density liquid (HDL) water.
  • Moderate confinement enabled homogeneous nucleation of water at 205 K, within the "no-man's land" region.
  • Hydrate formation in 1-propanol-rich mixtures linked to ultra-viscous water phases (HDL and low-density liquid).

Conclusions:

  • The study elucidates the intricate phase behavior of 1-propanol/water mixtures.
  • Confinement plays a critical role in the crystallization and dynamics of water within these mixtures.
  • The findings provide insights into the nature of ultra-viscous water and hydrate formation.