Phase equilibria of methane and carbon dioxide hydrates in the aqueous MgCl2 solutions

Kang, Seong-Pil; Chun, Moon-Kyoon; Lee, Huen

doi:10.1016/s0378-3812(98)00233-7

Cited by 118 publications

(96 citation statements)

References 13 publications

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“…Also noted by Prieto-Ballesteros et al (2005) is that the salt depresses the freezing point of water by approximately 4 K, and so a larger temperature difference between ice melting and clathrate dissociation is observed in the eutectic salt system. A similar trend was reported earlier by Kang et al (1998) who found that, as they increased the concentration of MgCl 2 , the amount of hydrate formed at a particular pressure becomes less. Fig.…”

Section: Inhibiting Effect Of Mgso 4 On Clathrate Formationsupporting

confidence: 89%

Properties of CO₂clathrate hydrates formed in the presence of MgSO₄solutions with implications for icy moons

Safi

Thompson

Evans

et al. 2017

A&A

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Context. There is evidence to suggest that clathrate hydrates have a significant effect on the surface geology of icy bodies in the Solar System. However the aqueous environments believed to be present on these bodies are likely to be saline rather than pure water. Laboratory work to underpin the properties of clathrate hydrates in such environments is generally lacking. Aims. We aim to fill this gap by carrying out a laboratory investigation of the physical properties of CO 2 clathrate hydrates produced in weak aqueous solutions of MgSO 4 . Methods. We use in situ synchrotron X-ray powder diffraction to investigate clathrate hydrates formed at high CO 2 pressure in ice that has formed from aqueous solutions of MgSO 4 with varying concentrations. We measure the thermal expansion, density and dissociation properties of the clathrates under temperature conditions similar to those on icy Solar System bodies. Results. We find that the sulphate solution inhibits the formation of clathrates by lowering their dissociation temperatures. Hysteresis is found in the thermal expansion coefficients as the clathrates are cooled and heated; we attribute this to the presence of the salt in solution. We find the density derived from X-ray powder diffraction measurements is temperature and pressure dependent. When comparing the density of the CO 2 clathrates to that of the solution in which they were formed, we conclude that they should sink in the oceans in which they form. We also find that the polymorph of ice present at low temperatures is Ih rather than the expected Ic, which we tentatively attribute to the presence of the MgSO 4 . Conclusions. We (1) conclude that the density of the clathrates has implications for their behaviour in satellite oceans as their sinking and floating capabilities are temperature and pressure dependent, (2) conclude that the presence of MgSO 4 inhibits the formation of clathrates and in some cases may even affect their structure and (3) report the dominance of Ih throughout the experimental procedure despite Ic being the stable phase at low temperature.

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Section: Inhibiting Effect Of Mgso 4 On Clathrate Formationsupporting

confidence: 89%

Properties of CO₂clathrate hydrates formed in the presence of MgSO₄solutions with implications for icy moons

Safi

Thompson

Evans

et al. 2017

A&A

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“…As shown in Figure 5 to Figure 8, the model can accurately predict the inhibition effect of salts on the hydrate stability conditions; good agreement with the data generated in this work is observed for both single and mixed electrolyte solutions. However, the published experimental data by Kang et al (1998) Water content of methane in equilibrium with liquid water. Experimental data at 273.11 K from Kosyakov et al, 1982 (•) and Althaus, 1999 (• •).…”

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confidence: 99%

Methane and Water Phase Equilibria in the Presence of Single and Mixed Electrolyte Solutions Using the Cubic-Plus-Association Equation of State

Haghighi

Chapoy

Tohidi

2008

Oil & Gas Science and Technology - Rev. IFP

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Résumé -Application de l'équation d'état Cubic-Plus-Association pour la prédiction des équilibres entre phases pour les systèmes contenant du méthane et de l'eau en présence d'électrolyte(s) -Les hydrates de méthane ont été largement présentés comme une potentielle nouvelle source d'énergie. Les hydrates à l'état naturel peuvent se former dans diverses roches ou sédiments si les conditions appropriées de pression et température en présence d'eau et de méthane sont réunies. Toutefois, la salinité des eaux de formation peut connaître d'importantes variations, et ces changements modifient la zone de stabilité des hydrates. En outre, l'eau de gisement produite avec les fluides de réservoir peut contenir diverses quantités de sels, pouvant prévenir la formation d'hydrates. Par conséquent, il est essentiel d'obtenir une meilleure compréhension de l'effet des sels sur la stabilité des hydrates. Dans cette communication, de nouvelles données expérimentales de dissociation d'hydrates de méthane en présence de solutions aqueuses contenant différentes concentrations de NaCl, KCl et de MgCl 2 ont été réalisées. Les nouvelles données ont été mesurées en utilisant une méthode à volume constant. La précision et la fiabilité des mesures expérimentales ont été démontrées en comparant les mesures avec les données de la littérature. Une approche thermodynamique dans lequel l'équation d'état CPA est combinée avec une modification du terme électrostatique proposé par Debye-Hückel a été employée pour modéliser les équilibres entre phases. Les conditions de formation d'hydrates sont modélisées par la théorie développée par van der Waals et Platteeuw. Pour modéliser en milieux poreux les équilibres entre phases d'hydrate, l'effet de la pression capillaire a été pris en compte. Les prédictions du modèle développé ont été validées par rapport à des données expérimentales indépendantes et les données obtenues dans ce travail. Un bon accord entre les prédictions et les données expérimentales a été observé, confirmant la fiabilité du modèle développé. Abstract -Methane and Water Phase Equilibria in the Presence of Single and Mixed Electrolyte

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“…Fig. 6 shows a comparison between the predictions of this method and experimental data [24] for the hydrate phase boundary of methane in the presence of MgCl 2 aqueous solutions. As can be observed, the AAN shows acceptable predictions even at higher concentrations of MgCl 2 used for developing this predictive method ( Table 1).…”

Section: Resultsmentioning

confidence: 99%

Predicting hydrate stability zones of petroleum fluids using sound velocity data of salt aqueous solutions

Mohammadi

Martínez-López

Richon

2007

Fluid Phase Equilibria

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Phase equilibria of methane and carbon dioxide hydrates in the aqueous MgCl2 solutions

Cited by 118 publications

References 13 publications

Properties of CO₂clathrate hydrates formed in the presence of MgSO₄solutions with implications for icy moons

Properties of CO₂clathrate hydrates formed in the presence of MgSO₄solutions with implications for icy moons

Methane and Water Phase Equilibria in the Presence of Single and Mixed Electrolyte Solutions Using the Cubic-Plus-Association Equation of State

Predicting hydrate stability zones of petroleum fluids using sound velocity data of salt aqueous solutions

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Phase equilibria of methane and carbon dioxide hydrates in the aqueous MgCl2 solutions

Cited by 118 publications

References 13 publications

Properties of CO2clathrate hydrates formed in the presence of MgSO4solutions with implications for icy moons

Properties of CO2clathrate hydrates formed in the presence of MgSO4solutions with implications for icy moons

Methane and Water Phase Equilibria in the Presence of Single and Mixed Electrolyte Solutions Using the Cubic-Plus-Association Equation of State

Predicting hydrate stability zones of petroleum fluids using sound velocity data of salt aqueous solutions

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Product

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Properties of CO₂clathrate hydrates formed in the presence of MgSO₄solutions with implications for icy moons

Properties of CO₂clathrate hydrates formed in the presence of MgSO₄solutions with implications for icy moons