Explorations of gas hydrate crystal growth by molecular simulations

Liang, Shuai; Kusalik, Peter G.

doi:10.1016/j.cplett.2010.05.088

Cited by 94 publications

(88 citation statements)

References 90 publications

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“…Owing to the important applications of natural gas hydrates, the interest to understand and quantify its properties has increased [9]. Thus, molecular-based theories and molecular simulations have been one of the main and growing areas of scientific development over the past decades [12][13][14][15][16][17][18][19][20]. Since water molecules exist in the hydrate lattice, for an exact description of the system, the strong electrostatic interactions have to be included [21,22].…”

Section: Introductionmentioning

confidence: 99%

The Wolf method applied to the type I methane and carbon dioxide gas hydrates

Sadeghifar

Dadvar

Karimi

et al. 2012

Journal of Molecular Graphics and Modelling

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Section: Introductionmentioning

confidence: 99%

The Wolf method applied to the type I methane and carbon dioxide gas hydrates

Sadeghifar

Dadvar

Karimi

et al. 2012

Journal of Molecular Graphics and Modelling

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“…1 Due to the crucial roles played by NGHs, many experimental and theoretical efforts have made to study these systems. [12][13][14][15][16][17][18] Experimentally, Raman, NMR, and other spectroscopic tools are the regular means to study NGHs. Especially, Raman spectroscopy has been used to identify the type of crystal phase, [19][20][21] type of guest molecule, 19 cage occupancy, 21 and hydration number, [21][22] to monitor the nucleation and growth processes in real-time, 23 to study phase transformations, [24][25] and to detect the location of NGH deposits.…”

Section: Introductionmentioning

confidence: 99%

C–C Stretching Raman Spectra and Stabilities of Hydrocarbon Molecules in Natural Gas Hydrates: A Quantum Chemical Study

Liu

Ojamäe

2014

J. Phys. Chem. A

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Abstract:The presence of specific hydrocarbon gas molecules in various types of water cavities in natural gas hydrates (NGHs) are governed by the relative stabilities of these encapsulated guest molecule ─ water cavity combinations. Using molecular quantum-chemical dispersion-corrected hybrid density functional computations, the interaction energies (ΔEhost-guest) and cohesive energies (ΔEcoh), enthalpies and Gibbs free energies for the complexes of host water cages and hydrocarbon guest molecules are calculated at the ωB97X-D/6-311++G(2d,2p) level of theory. The zero point energy effect of ΔEhost-guest and ΔEcoh is found to be quite substantial. The energetically optimal host-guest combinations for seven hydrocarbon gas molecules (CH4, C2H6, C3H6, C3H8, C4H8, i-C4H10, and n-C4H10) and various water cavities (D, ID, T, P, H and I) in NGHs are found to be CH4@D, C2H6@T, C3H6@T, C3H8@T, C4H8@T/P/H, i-C4H10@H, and n-C4H10@H, as the largest cohesive energy magnitudes will be obtained with these host-guest combinations. The stabilities of various water cavities enclosing hydrocarbon molecules are evaluated from the computed cohesive Gibbs free energies: CH4 prefer to be trapped in a ID cage; C2H6 prefer T cages; C3H6 and C3H8 prefer T and H cages; C4H8 and i-C4H10 prefer H cages; and n-C4H10 prefer I cages. The vibrational frequencies and Raman intensities of the C-C stretching vibrational modes for these seven hydrocarbon molecules enclosed in each water cavity are computed. A blue shift results after the guest molecule is trapped from gas phase into various water cages due to the host-guest interactions between the water cage and hydrocarbon molecule. The frequency shifts to the red as the radius of water cages increases. The model calculations support the view that C-C stretching vibrations of hydrocarbon molecules in the water cavities can be used as a tool to identify the types of crystal phases and guest molecules in NGHs.2

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“…Crystal-like molecules are thereby defined as those having their orientations within a certain threshold value from the orientations of the molecules from the relaxed unit cell used to construct the crystal (called reference orientations) and at least one neighbor among the crystal molecules, as described in detail in our papers [40,51]. However, the identification of an appropriate set of order parameters can be far from trivial in many other cases [107], and a significant number of approaches to differentiate one state from the other can be found in the literature [12,20,33,[96][97][98][108][109][110][111][112][113][114][115][116][117].…”

Section: Linking Nanoscale and Microscalementioning

confidence: 99%

“…Most investigations of crystallization processes using MD consider the distinct faces of the crystal in contact with the solvent [11,12,[14][15][16]33,35,[96][97][98]. However, time scales accessible in regular MD simulation are often not sufficient to resolve dissolution from the perfectly flat interfaces.…”

Section: Superiority Of Three-dimensional Over Two-dimensional Dissolmentioning

confidence: 99%

In Silico Prediction of Growth and Dissolution Rates for Organic Molecular Crystals: A Multiscale Approach

2017

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Solution crystallization and dissolution are of fundamental importance to science and industry alike and are key processes in the production of many pharmaceutical products, special chemicals, and so forth. The ability to predict crystal growth and dissolution rates from theory and simulation alone would be of a great benefit to science and industry but is greatly hindered by the molecular nature of the phenomenon. To study crystal growth or dissolution one needs a multiscale simulation approach, in which molecular-level behavior is used to parametrize methods capable of simulating up to the microscale and beyond, where the theoretical results would be industrially relevant and easily comparable to experimental results. Here, we review the recent progress made by our group in the elaboration of such multiscale approach for the prediction of growth and dissolution rates for organic crystals on the basis of molecular structure only and highlight the challenges and future directions of methodic development.

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Explorations of gas hydrate crystal growth by molecular simulations

Cited by 94 publications

References 90 publications

The Wolf method applied to the type I methane and carbon dioxide gas hydrates

The Wolf method applied to the type I methane and carbon dioxide gas hydrates

C–C Stretching Raman Spectra and Stabilities of Hydrocarbon Molecules in Natural Gas Hydrates: A Quantum Chemical Study

In Silico Prediction of Growth and Dissolution Rates for Organic Molecular Crystals: A Multiscale Approach

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