On the thermodynamic stability of hydrogen clathrate hydrates

Keisuke Katsumasa, Kenichiro Koga, Hideki Tanaka

Research output: Contribution to journalArticle

58 Citations (Scopus)

Abstract

The cage occupancy of hydrogen clathrate hydrate has been examined by grand canonical Monte Carlo (GCMC) simulations for wide ranges of temperature and pressure. The simulations are carried out with a fixed number of water molecules and a fixed chemical potential of the guest species so that hydrogen molecules can be created or annihilated in the clathrate. Two types of the GCMC simulations are performed; in one the volume of the clathrate is fixed and in the other it is allowed to adjust itself under a preset pressure so as to take account of compression by a hydrostatic pressure and expansion due to multiple cage occupancy. It is found that the smaller cage in structure II is practically incapable of accommodating more than a single guest molecule even at pressures as high as 500 MPa, which agrees with the recent experimental investigations. The larger cage is found to encapsulate at most 4 hydrogen molecules, but its occupancy is dependent significantly on the pressure of hydrogen.

Original languageEnglish
Article number044509
JournalThe Journal of Chemical Physics
Volume127
Issue number4
DOIs
Publication statusPublished - 2007

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clathrates
Hydrates
hydrates
Hydrogen
Thermodynamic stability
thermodynamics
Molecules
hydrogen
molecules
simulation
Chemical potential
Hydrostatic pressure
hydrostatic pressure
expansion
Water
water
Temperature
temperature
Monte Carlo simulation

ASJC Scopus subject areas

  • Atomic and Molecular Physics, and Optics

Cite this

On the thermodynamic stability of hydrogen clathrate hydrates. / Katsumasa, Keisuke; Koga, Kenichiro; Tanaka, Hideki.

In: The Journal of Chemical Physics, Vol. 127, No. 4, 044509, 2007.

Research output: Contribution to journalArticle

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