Simulation of the carbon dioxide hydrate-water interfacial energy

Algaba, Jesús; Acuña, Esteban; Mı́guez, José Manuel; Mendiboure, Bruno; Zerón, Iván M.; Blas, Felipe J.

doi:10.1016/j.jcis.2022.05.029

Cited by 14 publications

(5 citation statements)

References 102 publications

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“…The value found here for the planar interface for the methane hydrate seems to be higher than the value found by Anderson et al, 132 which is equal to 32 mJ/m 2 and the value of about 29-30 mJ/m 2 found recently for carbon dioxide hydrate 133,134 at T 3 and 400 bars. It would be interesting to determine in the future the value of γ of the methane hydrate by using mold integration 135 for the models of water and methane used in this work (as it has been done recently for the carbon dioxide hydrate 133,134 ) to confirm the larger value of γ suggested by the results of this work.…”

Section: Fig 13contrasting

confidence: 78%

Homogeneous nucleation rate of methane hydrate formation under experimental conditions from seeding simulations

Grabowska

Blazquez

Sanz

et al. 2023

The Journal of Chemical Physics

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In this work, we shall estimate via computer simulations the homogeneous nucleation rate for the methane hydrate at 400 bars for a supercooling of about 35 K. The TIP4P/ICE model and a Lennard-Jones center were used for water and methane, respectively. To estimate the nucleation rate, the seeding technique was employed. Clusters of the methane hydrate of different sizes were inserted into the aqueous phase of a two-phase gas–liquid equilibrium system at 260 K and 400 bars. Using these systems, we determined the size at which the cluster of the hydrate is critical (i.e., it has 50% probability of either growing or melting). Since nucleation rates estimated from the seeding technique are sensitive to the choice of the order parameter used to determine the size of the cluster of the solid, we considered several possibilities. We performed brute force simulations of an aqueous solution of methane in water in which the concentration of methane was several times higher than the equilibrium concentration (i.e., the solution was supersaturated). From brute force runs, we infer the value of the nucleation rate for this system rigorously. Subsequently, seeding runs were carried out for this system, and it was found that only two of the considered order parameters were able to reproduce the value of the nucleation rate obtained from brute force simulations. By using these two order parameters, we estimated the nucleation rate under experimental conditions (400 bars and 260 K) to be of the order of log10 ( J/(m3 s)) = −7(5).

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Section: Fig 13contrasting

confidence: 78%

Homogeneous nucleation rate of methane hydrate formation under experimental conditions from seeding simulations

Grabowska

Blazquez

Sanz

et al. 2023

The Journal of Chemical Physics

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“…For this purpose, we shall use the order parameter proposed by Lechner and Dellago . We found that was a reasonable order parameter (notice that for ice Ih we used , but this is not a good order parameter for hydrate formation, as noted by Algaba et al). While may not be the optimal order parameter, as many other choices have been proposed for hydrates, − it is reasonable, simple, and adequate for our purpose of detecting molecules of the solid phase.…”

Section: Methodsmentioning

confidence: 90%

Solubility of Methane in Water: Some Useful Results for Hydrate Nucleation

et al. 2022

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In this paper, the solubility of methane in water along the 400 bar isobar is determined by computer simulations using the TIP4P/Ice force field for water and a simple LJ model for methane. In particular, the solubility of methane in water when in contact with the gas phase and the solubility of methane in water when in contact with the hydrate has been determined. The solubility of methane in a gas–liquid system decreases as temperature increases. The solubility of methane in a hydrate–liquid system increases with temperature. The two curves intersect at a certain temperature that determines the triple point T 3 at a certain pressure. We also determined T 3 by the three-phase direct coexistence method. The results of both methods agree, and we suggest 295(2) K as the value of T 3 for this system. We also analyzed the impact of curvature on the solubility of methane in water. We found that the presence of curvature increases the solubility in both the gas–liquid and hydrate–liquid systems. The change in chemical potential for the formation of hydrate is evaluated along the isobar using two different thermodynamic routes, obtaining good agreement between them. It is shown that the driving force for hydrate nucleation under experimental conditions is higher than that for the formation of pure ice when compared at the same supercooling. We also show that supersaturation (i.e., concentrations above those of the planar interface) increases the driving force for nucleation dramatically. The effect of bubbles can be equivalent to that of an additional supercooling of about 20 K. Having highly supersaturated homogeneous solutions makes possible the spontaneous formation of the hydrate at temperatures as high as 285 K (i.e., 10K below T 3). The crucial role of the concentration of methane for hydrate formation is clearly revealed. Nucleation of the hydrate can be either impossible or easy and fast depending on the concentration of methane which seems to play the leading role in the understanding of the kinetics of hydrate formation.

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“…To date, the Mold Integration method has been widely used to calculate solid-liquid interfacial free energy of hard spheres (Espinosa et al, 2014), pseudo-hard spheres (Sanchez-Burgos, Sanz, et al, 2021), Lennard-Jones (Espinosa et al, 2014), SPC/E water with JC NaCl (Sanchez-Burgos & Espinosa, 2023), NaCl (Tosi-Fumi) (Espinosa et al, 2015), ice-water interfaces for TIP4P, TPI4P/2005 TIP4P/Ice and mW models , and CO 2 hydrate water interfacial energy (Algaba et al, 2022;Romero-Guzmán et al, 2023;Zerón et al, 2022). The Lattice Mold method has been used to calculate the nucleation rate of pseudo-hard spheres and NaCl from its melt (Espinosa, Sampedro, et al, 2016), and mW and TIP4P/Ice water models (Sanchez-Burgos et al, 2022).…”

Section: Scientific Backgroundmentioning

confidence: 99%

Mold: a LAMMPS package to compute interfacial free energies and nucleation rates

Tejedor,

Sanchez-Burgos,

Sanz

et al. 2024

JOSS

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The determination of the free energy cost of forming an interface between two phases, i.e. the interfacial free energy, is critical for characterizing a phase transition. In the particular case of liquid-to-solid transitions, it is not straightforward to obtain this quantity through experiment or computation. Here, we present the computational package Mold, which is integrated in the Molecular Dynamics open-source software LAMMPS (Thompson et al., 2022). Mold enables direct calculation of the interfacial free energy between arbitrarily complex crystal structures and liquids/solutions at coexistence conditions through the Mold Integration method (Espinosa et al., 2014). Furthermore, the extension of this method for determining crystal nucleation rates-the probablity of a critical nucleus to emerge per unit of volume and time within a metastable phase-is also incorporated in the package, termed Lattice Mold method (Espinosa, Sampedro, et al., 2016). Altogether, we detail here the required codes, scripts, and instructions for evaluating the two most challenging quantities determining the feasibility of a liquid-to-solid transition, implemented to work alongside the MD package LAMMPS.

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Simulation of the carbon dioxide hydrate-water interfacial energy

Cited by 14 publications

References 102 publications

Homogeneous nucleation rate of methane hydrate formation under experimental conditions from seeding simulations

Homogeneous nucleation rate of methane hydrate formation under experimental conditions from seeding simulations

Solubility of Methane in Water: Some Useful Results for Hydrate Nucleation

Mold: a LAMMPS package to compute interfacial free energies and nucleation rates

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