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Phase Equilibria of the CH 4 -CO 2 Binary and the CH 4 -CO 2 -H 2 O Ternary Mixtures in the Presence of a CO 2 -Rich Liquid Phase

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  • Ludovic Nicolas Legoix

    (GEOMAR, Helmholtz Centre for Ocean Research Kiel, Wischhofstr. 1-3, D-24148 Kiel, Germany
    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)

  • Livio Ruffine

    (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)

  • Jean-Pierre Donval

    (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)

  • Matthias Haeckel

    (GEOMAR, Helmholtz Centre for Ocean Research Kiel, Wischhofstr. 1-3, D-24148 Kiel, Germany)

Abstract

The knowledge of the phase behavior of carbon dioxide (CO 2 )-rich mixtures is a key factor to understand the chemistry and migration of natural volcanic CO 2 seeps in the marine environment, as well as to develop engineering processes for CO 2 sequestration coupled to methane (CH 4 ) production from gas hydrate deposits. In both cases, it is important to gain insights into the interactions of the CO 2 -rich phase—liquid or gas—with the aqueous medium (H 2 O) in the pore space below the seafloor or in the ocean. Thus, the CH 4 -CO 2 binary and CH 4 -CO 2 -H 2 O ternary mixtures were investigated at relevant pressure and temperature conditions. The solubility of CH 4 in liquid CO 2 (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 k ij (CH 4 -CO 2 ) = 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 CO 2 -rich fluid phase in the presence of H 2 O. In contrast to the behavior in the presence of vapor, gas hydrates become more stable when increasing the CH 4 content, and the relative proportion of CH 4 to CO 2 decreases in the CO 2 -rich phase after gas hydrate formation.

Suggested Citation

  • Ludovic Nicolas Legoix & Livio Ruffine & Jean-Pierre Donval & Matthias Haeckel, 2017. "Phase Equilibria of the CH 4 -CO 2 Binary and the CH 4 -CO 2 -H 2 O Ternary Mixtures in the Presence of a CO 2 -Rich Liquid Phase," Energies, MDPI, vol. 10(12), pages 1-11, December.
    • Handle: RePEc:gam:jeners:v:10:y:2017:i:12:p:2034-:d:121372
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    References listed on IDEAS

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    1. Christian Deusner & Nikolaus Bigalke & Elke Kossel & Matthias Haeckel, 2012. "Methane Production from Gas Hydrate Deposits through Injection of Supercritical CO 2," Energies, MDPI, vol. 5(7), pages 1-29, June.
    2. Judith M. Schicks & Erik Spangenberg & Ronny Giese & Bernd Steinhauer & Jens Klump & Manja Luzi, 2011. "New Approaches for the Production of Hydrocarbons from Hydrate Bearing Sediments," Energies, MDPI, vol. 4(1), pages 1-22, January.
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    1. Ludovic Nicolas Legoix & Livio Ruffine & Christian Deusner & Matthias Haeckel, 2018. "Experimental Study of Mixed Gas Hydrates from Gas Feed Containing CH 4 , CO 2 and N 2 : Phase Equilibrium in the Presence of Excess Water and Gas Exchange," Energies, MDPI, vol. 11(8), pages 1-12, July.

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