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Competitive cage occupancy of hydrogen and argon in structure-II hydrates
Authors:Shingo Amano  Takaaki TsudaShunsuke Hashimoto  Takeshi SugaharaKazunari Ohgaki
Affiliation:Division of Chemical Engineering, Department of Materials Engineering Science, Graduate School of Engineering Science, Osaka University, 1-3 Machikaneyama, Toyonaka, Osaka 560-8531, Japan
Abstract:The cage occupancy of hydrogen in the single-crystals of simple hydrogen hydrates and hydrogen + argon mixed-gas hydrates was investigated by means of in situ Raman spectroscopy under the three-phase (hydrate + water + fluid) equilibrium condition. In the equilibrium pressure region higher than approximately 25 MPa, four hydrogen cluster and argon competitively occupied the large cages of structure-II hydrogen + argon mixed-gas hydrates. In addition, Raman spectroscopic analysis at liquid nitrogen temperature (77 K) supports that the clusters of two, three, or four hydrogen molecules occupy large cages.
Keywords:Gas hydrate   Hydrogen   Raman spectroscopy   Cage occupancy   High pressure
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