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Low barriers for hydrogen diffusion in sII clathrate.

Thuat T Trinh1, Magnus H Waage, Titus S van Erp

  • 1Department of Chemistry, Norwegian University of Science and Technology, Høgskoleringen 5, 7491-Trondheim, Norway. Signe.Kjelstrup@ntnu.no.

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Gas diffusion in hydrates is poorly understood. New simulations show that cage occupancy and water lattice flexibility explain experimental hydrogen diffusion rates in sII hydrates, with low energy barriers.

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Area of Science:

  • Materials Science
  • Physical Chemistry
  • Chemical Engineering

Background:

  • Gas molecule transport in hydrates remains poorly understood.
  • A discrepancy exists between experimental and computed diffusion constants for hydrogen guests in sII hydrates.

Purpose of the Study:

  • To explain the experimentally observed diffusion rates of hydrogen in sII hydrates.
  • To reconcile the mismatch between experimental and computational diffusion data.

Main Methods:

  • Density Functional Theory (DFT)-based molecular dynamics simulations were employed.
  • Simulations were conducted at a temperature of 100 K.
  • The influence of cage occupancy and water lattice flexibility was investigated.

Main Results:

  • Barriers for hydrogen diffusion between cages were found to be as low as 5 kJ mol(-1).
  • These calculated barriers closely match experimentally observed values.
  • The study highlights the importance of cage occupancy and lattice flexibility.

Conclusions:

  • The study provides a clear explanation for experimentally observed hydrogen diffusion rates in sII hydrates.
  • The findings reconcile discrepancies between experimental and computational diffusion data.
  • This work advances the understanding of gas transport mechanisms in clathrate hydrates.