Phase relations and binary clathrate hydrate formation in the system H 2-THF-H2O

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Abstract

Experimentally determined equilibrium phase relations are reported for the system H2-THF-H2O as a function of aqueous tetrahydrofuran (THF) concentration from 260 to 290 K at pressures up to 45 MPa. Data are consistent with the formation of cubic structure-II (CS-II) binary H 2-THF clathrate hydrates with a stoichiometric THF-to-water ratio of 1:17, which can incorporate modest volumes of molecular hydrogen at elevated pressures. Direct compositional analyses of the clathrate phase, at both low (0.20 mol %) and stoichiometric (5.56 mol %) initial THF aqueous concentrations, are consistent with observed phase behavior, suggesting full occupancy of large hexakaidecahedral (51264) clathrate cavities by THF, coupled with largely complete (80-90%) filling of small dodecahedral (5 12) cages by single H2 molecules at pressures of >30 MPa, giving a clathrate formula of (H2) =2·THF·17H2O. Results should help to resolve the current controversy over binary H2-THF hydrate hydrogen contents; data confirm recent reports that suggest a maximum of ~1 mass % H2, this contradicting values of up to 4 mass % previously claimed for comparable conditions. © 2007 American Chemical Society.

Original languageEnglish
Pages (from-to)3440-3444
Number of pages5
JournalLangmuir
Volume23
Issue number6
DOIs
Publication statusPublished - 13 Mar 2007

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