Cage occupancies in the high pressure structure H methane hydrate: A neutron diffraction study

Tulk, Christopher A.; Klug, Dennis D.; Moreira Dos Santos, Antonio F.; Karotsis, Georgios; Guthrie, Malcolm; Molaison, Jamie J.; Pradhan, Neelam

doi:10.1063/1.3679875

Title: Cage occupancies in the high pressure structure H methane hydrate: A neutron diffraction study

Journal Article · Wed Feb 01 00:00:00 EST 2012 · The Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.3679875· OSTI ID:1034701

^[1]; Klug, Dennis D. ^[2];

^[1]; Karotsis, Georgios ^[1]; Guthrie, Malcolm ^[3];

^[1]; Pradhan, Neelam ^[1]

ORNL
National Research Council of Canada
Carnegie Institution of Washington

A neutron diffraction study was performed on the CD4 : D2O structure H clathrate hydrate to refine its CD4 fractional cage occupancies. Samples of ice VII and hexagonal (sH) methane hydrate were produced in a Paris–Edinburgh press and in situ neutron diffraction data collected. The data were analyzed with the Rietveld method and yielded average cage occupancies of 3.1 CD4 molecules in the large 20-hedron (51268) cages of the hydrate unit cell. Each of the pentagonal dodecahedron (512) and 12-hedron (435663) cages in the sH unit cell are occupied with on average 0.89 and 0.90 CD4 molecules, respectively. This experiment avoided the co-formation of Ice VI and sH hydrate, this mixture is more difficult to analyze due to the proclivity of ice VI to form highly textured crystals, and overlapping Bragg peaks of the two phases. These results provide essential information for the refinement of intermolecular potential parameters for the water–methane hydrophobic interaction in clathrate hydrates and related dense structures

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-00OR22725

OSTI ID:: 1034701

Journal Information:: The Journal of Chemical Physics, Vol. 136, Issue 5; ISSN 0021-9606

Country of Publication:: United States

Language:: English

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Title: Cage occupancies in the high pressure structure H methane hydrate: A neutron diffraction study

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