Monte Carlo simulation studies of clathrate hydrates: A review

Engineering Model for Predicting the Intradiffusion Coefficients of Hydrogen and Oxygen in Vapor, Liquid, and Supercritical Water based on Molecular Dynamics Simulations

“…For modeling H 2 , the single-site force fields developed by Buch, Vrabec and co-workers, and Hirschfelder et al, the two-site force field by Cracknell, and the modified three-site Silvera–Goldman by Alavi et al, and Marx and Nielaba force fields are tested (for brevity these force fields are referred to as Buch, Vrabec, Hirschfelder, Cracknell, Silvera–Goldman, and Marx hereafter). These H 2 force fields have been recently used in the literature to predict the thermophysical properties of H 2 O/H 2 mixtures in a wide range of temperatures and pressures. ,, Furthermore, the modified Silvera–Goldman force field has been used extensively in MD , and Monte Carlo − studies related to H 2 storage in clathrate hydrate structures. For additional information on the performance of the H 2 force fields for various mixtures, conditions, and properties, the reader is referred to the recent studies by Yang et al and Bartolomeu et al , For O 2 , the two-site force fields developed by Bohn et al., Miyano, and Coon et al, and the three-site models developed by Hansen et al, Vrabec et al, and Watanabe are used (for brevity these force fields are referred to as Bohn, Miyano, Coon, Hansen, Vrabec, and Watanabe hereafter).…”

Molecular Selectivity of CH4–C2H6 Mixed Hydrates: A GCMC Study

“…Again, this raises the question of the transferability of some parameters to thermodynamic conditions different from those where they have been fitted . More recently, computer simulations based on an atomic-scale description of the systems under consideration have appeared as a promising tool to characterize the composition and the stability of clathrates. , In this respect, calculations performed on the grand canonical (μ, V , T ) ensemble, where the number of trapped molecules can vary in the simulations, is a particularly suitable tool for characterizing the fraction of the enclathrated gases in the different types of cages, which is one of the most important sought after data. Indeed, in the grand canonical Monte Carlo (GCMC) simulations, the chemical potential rather than the number of the molecules is fixed and thus, the number of enclathrated molecules can be calculated, as a function of their chemical potential or of their partial pressure.…”

“…Indeed, in the grand canonical Monte Carlo (GCMC) simulations, the chemical potential rather than the number of the molecules is fixed and thus, the number of enclathrated molecules can be calculated, as a function of their chemical potential or of their partial pressure. Notice that this numerical method can be used for single-guest clathrate as well as to characterize the fractional occupancy of multiple-guest clathrates . Thus, we have recently performed GCMC simulations to characterize ammonia enclathration under conditions relevant to astrophysical environments, and to thoroughly investigate the composition of the multiple-guest clathrate formed in contact with a gas mixture of CO and N 2 , at very low temperatures (typically around 50 K) in the context of the comet 67P/Churyumov–Gerasimenko .…”

“…Notice that this numerical method can be used for single-guest clathrate as well as to characterize the fractional occupancy of multiple-guest clathrates. 18 Thus, we have recently performed GCMC simulations to characterize ammonia enclathration under conditions relevant to astrophysical environments, 20 and to thoroughly investigate the composition of the multiple-guest clathrate formed in contact with a gas mixture of CO and N 2 , at very low temperatures (typically around 50 K) in the context of the comet 67P/Churyumov−Gerasimenko. 21 In addition, the results of GCMC simulations performed at higher temperatures up to 150 K, have been shown to agree fairly well with recently available measured data, especially when regarding the clathrate selectivity which appeared to strongly favor CO at the expense of N 2 trapping.…”

Molecular Simulations of CO2/CH4, CO2/N2 and N2/CH4 Binary Mixed Hydrates

“…A molecular-level insight into the mechanism of competitive cage occupancy in gas hydrate can be obtained from molecular simulation studies. However, despite the successful application of molecular dynamics and Monte Carlo simulation techniques to one-component hydrates, including those of CH 4 , CO 2 , and N 2 , there is only a very limited number of simulation studies considering the properties of mixed hydrates [20][21][22]. A comparison of molecular dynamics simulation data for one-component CH 4 and CO 2 hydrates and CH 4 /CO 2 mixed hydrate suggests that the latter species may be more stable than either of the one-component gas hydrates [23].…”