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AuthorAtilhan, Mert
AuthorPala, Nezih
AuthorAparicio, Santiago
Available date2016-05-16T10:55:22Z
Publication Date2014-03
Publication NameJournal of Molecular Modeling
CitationAtilhan, M., Pala, N., Aparicio, S. "A quantum chemistry study of natural gas hydrates" (2014) Journal of Molecular Modeling, 20 (4), art. no. 2182, .
ISSN1610-2940
URIhttp://dx.doi.org/10.1007/s00894-014-2182-z
URIhttp://hdl.handle.net/10576/4520
AbstractThe structure and properties of natural gas hydrates containing hydrocarbons, CO2, and N2 molecules were studied by using computational quantum chemistry methods via the density functional theory approach. All host cages involved in I, II, and H types structures where filled with hydrocarbons up to pentanes, CO2 and N2 molecules, depending on their size, and the structures of these host-guest systems optimized. Structural properties, vibrational spectra, and density of states were analyzed together with results from atoms-in-a-molecule and natural bond orbitals methods. The inclusion of dispersion terms in the used functional plays a vital role for obtaining reliable information, and thus, B97D functional was shown to be useful for these systems. Results showed remarkable interaction energies, not strongly affected by the type of host cage, with molecules tending to be placed at the center of the cavities when host cages and guest molecules cavities are of similar size, but with molecules approaching hexagonal faces for larger cages. Vibrational properties show remarkable features in certain regions, with shiftings rising from host-guest interactions, and useful patterns in the terahertz region rising from water surface vibrations strongly coupled with guest molecules. Likewise, calculations on crystal systems for the I and H types were carried out using a pseudopotential approach combined with Grimme's method to take account of dispersion.
SponsorNPRP grant (National Priorities Research Program, No: 09-1211-2-475, Integrated Terahertz Technologies for Methane Gas Production from Clathrates and Real Time Analysis) from the Qatar National Research Fund. We also thank National Energy Research Scientific Computing Center (NERSC, Department of Energy, USA) for providing Supercomputing Facilities under project #86124.
Languageen
PublisherSpringer Verlag
SubjectDensity functional theory
SubjectHydrates
SubjectNatural gas
SubjectQuantumchemistry
TitleA quantum chemistry study of natural gas hydrates
TypeArticle
Issue Number4
Volume Number20


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