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Can clathrates heterogeneously nucleate ice?

Matías H Factorovich1, Pavithra M Naullage1, Valeria Molinero1

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The Journal of Chemical Physics
|September 23, 2019
PubMed
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Methane hydrates self-preserve via ice coating. This study reveals ice nucleates homogeneously from supercooled water at the clathrate interface, not heterogeneously, clarifying hydrate stability mechanisms.

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Area of Science:

  • Materials Science
  • Physical Chemistry
  • Geophysics

Background:

  • Methane hydrates exhibit anomalous self-preservation at ambient pressure when stored at 240–270 K.
  • This preservation is attributed to an ice coating preventing gas loss, but the ice nucleation mechanism remains unclear.

Purpose of the Study:

  • Investigate ice nucleation mechanisms on decomposing clathrate hydrates.
  • Determine if nucleation is heterogeneous (clathrate/vapor or clathrate/liquid interfaces) or homogeneous (supercooled water).

Main Methods:

  • Molecular simulations
  • Thermodynamic analysis
  • Nucleation theory
  • Contact angle measurements

Main Results:

  • Clathrates do not heterogeneously nucleate ice.
  • Ice nucleation occurs homogeneously due to cooling at the clathrate/liquid interface.
  • Weak epitaxy observed between sII clathrate (111) face and ice planes.
  • Interfacial free energy of the most favorable ice-clathrate interface determined as 59 ± 5 mJ/m².

Conclusions:

  • Homogeneous nucleation is the dominant mechanism for ice formation on decomposing methane hydrates.
  • Understanding this mechanism is crucial for managing gas hydrate stability and storage.
  • Results provide insights into gas clathrate formation at ice/vapor interfaces.