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Energies 2017, 10(12), 2034; doi:10.3390/en10122034

Phase Equilibria of the CH4-CO2 Binary and the CH4-CO2-H2O Ternary Mixtures in the Presence of a CO2-Rich Liquid Phase

1
GEOMAR, Helmholtz Centre for Ocean Research Kiel, Wischhofstr. 1-3, D-24148 Kiel, Germany
2
Institut Français de Recherche pour l’Exploitation de la Mer (IFREMER), Centre de Bretagne, Département Ressources physiques et Ecosystèmes de fond de Mer, Unité des Géosciences Marines, BP70, 29280 Plouzané, France
*
Authors to whom correspondence should be addressed.
Received: 20 September 2017 / Revised: 27 November 2017 / Accepted: 28 November 2017 / Published: 2 December 2017
(This article belongs to the Section Energy Fundamentals and Conversion)
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Abstract

The knowledge of the phase behavior of carbon dioxide (CO2)-rich mixtures is a key factor to understand the chemistry and migration of natural volcanic CO2 seeps in the marine environment, as well as to develop engineering processes for CO2 sequestration coupled to methane (CH4) production from gas hydrate deposits. In both cases, it is important to gain insights into the interactions of the CO2-rich phase—liquid or gas—with the aqueous medium (H2O) in the pore space below the seafloor or in the ocean. Thus, the CH4-CO2 binary and CH4-CO2-H2O ternary mixtures were investigated at relevant pressure and temperature conditions. The solubility of CH4 in liquid CO2 (vapor-liquid equilibrium) was determined in laboratory experiments and then modelled with the Soave–Redlich–Kwong equation of state (EoS) consisting of an optimized binary interaction parameter kij(CH4-CO2) = 1.32 × 10−3 × T − 0.251 describing the non-ideality of the mixture. The hydrate-liquid-liquid equilibrium (HLLE) was measured in addition to the composition of the CO2-rich fluid phase in the presence of H2O. In contrast to the behavior in the presence of vapor, gas hydrates become more stable when increasing the CH4 content, and the relative proportion of CH4 to CO2 decreases in the CO2-rich phase after gas hydrate formation. View Full-Text
Keywords: gas hydrate; CH4; CO2-rich mixtures; phase equilibria; Soave–Redlich–Kwong (SRK) cubic equation of state (EoS) gas hydrate; CH4; CO2-rich mixtures; phase equilibria; Soave–Redlich–Kwong (SRK) cubic equation of state (EoS)
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MDPI and ACS Style

Legoix, L.N.; Ruffine, L.; Donval, J.-P.; Haeckel, M. Phase Equilibria of the CH4-CO2 Binary and the CH4-CO2-H2O Ternary Mixtures in the Presence of a CO2-Rich Liquid Phase. Energies 2017, 10, 2034.

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