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Structural characterization of eutectic aqueous NaCl solutions under variable temperature and pressure conditions.

A-A Ludl1, L E Bove, A M Saitta

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Amorphous sodium chloride (NaCl) solutions under pressure exhibit structural changes, with hydration shells forming octahedra that break down at higher pressures. Unlike pure water, NaCl solutions do not show polyamorphism.

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Area of Science:

  • Materials Science
  • Physical Chemistry
  • Computational Physics

Background:

  • Amorphous solid water (e-HDA) exhibits polyamorphism, a phenomenon not yet fully understood.
  • The structural behavior of amorphous salt solutions under pressure remains an active area of research.

Purpose of the Study:

  • To investigate the pressure-induced structural evolution of amorphous sodium chloride (NaCl) solutions.
  • To validate a new polarizable force field for NaCl solutions under non-ambient conditions.
  • To explore the role of water's tetrahedral structure in polyamorphism.

Main Methods:

  • Combined neutron diffraction experiments and classical molecular dynamics simulations.
  • Studied amorphous NaCl solutions at pressures up to 4 GPa.
  • Measured the static structure factor as a function of pressure.

Main Results:

  • Amorphous NaCl solutions amorphize into a dense phase similar to e-HDA at ambient pressure.
  • Hydration shells around Na(+) cations initially form well-defined octahedra, which become irregular with increasing pressure.
  • No polyamorphic transition was observed in NaCl solutions under pressure.

Conclusions:

  • The absence of polyamorphism in NaCl solutions suggests it is dependent on the tetrahedral structure of water.
  • The validated force field provides a reliable tool for simulating salt solutions under pressure.
  • Structural changes in amorphous NaCl solutions are pressure-dependent, affecting cation hydration shells.