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  • 1
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    Phase Equilibria of the CH4-CO2 Binary and the CH4-CO2-H2O Ternary Mixtures in the Presence of a CO2-Rich Liquid Phase (2017)
    MDPI
    In:  Energies, 10 (12, Art. No. 2034).
    Details
    Publication Date: 2020-02-06
    Description: 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.
    Type: Article , PeerReviewed
    Format: text
    DOI: 10.3390/en10122034
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    OceanRep: Article in a Scientific Journal - peer-reviewed
  • 2
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    Experimental Study of Mixed Gas Hydrates from Gas Feed Containing CH4, CO2 and N2: Phase Equilibrium in the Presence of Excess Water and Gas Exchange (2018)
    MDPI
    In:  Energies, 11 (8). Art.Nr. 1984.
    Details
    Publication Date: 2021-03-18
    Description: This article presents gas hydrate experimental measurements for mixtures containing methane (CH4), carbon dioxide (CO2) and nitrogen (N2) with the aim to better understand the impact of water (H2O) on the phase equilibrium. Some of these phase equilibrium experiments were carried out with a very high water-to-gas ratio that shifts the gas hydrate dissociation points to higher pressures. This is due to the significantly different solubilities of the different guest molecules in liquid H2O. A second experiment focused on CH4-CO2 exchange between the hydrate and the vapor phases at moderate pressures. The results show a high retention of CO2 in the gas hydrate phase with small pressure variations within the first hours. However, for our system containing 10.2 g of H2O full conversion of the CH4 hydrate grains to CO2 hydrate is estimated to require 40 days. This delay is attributed to the shrinking core effect, where initially an outer layer of CO2-rich hydrate is formed that effectively slows down the further gas exchange between the vapor phase and the inner core of the CH4-rich hydrate grain.
    Type: Article , PeerReviewed
    Format: text
    DOI: 10.3390/en11081984
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    OceanRep: Article in a Scientific Journal - peer-reviewed
  • 3
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    Thermo-Hydro-Chemo-Mechanical Formulation for CH4-CO2 Hydrate Conversion Based on Hydrate Formation and Dissociation in Hydrate-Bearing Sediments (2016)
    ASCE
    In:  In: Geo-Chicago 2016. Geotechnical Special Publication, 270 . ASCE, New York, pp. 235-244. ISBN 978-0-7844-8013-7
    Details
    Publication Date: 2017-03-22
    Description: Gas production from gas hydrate-bearing sediments has been attracting global interests because of its potential to meet growing energy demand. Methane (CH4) gas can be extracted from CH4 hydrates by depressurization, thermal stimulation or chemical activation. However, it has never been produced on a commercial scale and the past field trials faced premature termination due to the technical difficulties such as excessive sand flow into the well, a phenomenon known as sand production. One exception is the trial at the Ignik Sikumi, Alaska in 2012, which was conducted by chemical activation followed by depressurization. During the trial, initial sand production ceased after two weeks while CH4 gas production continued for five weeks. The mitigation of sand production is deemed attributed to mechanical or hydraulic effects through formation of CO2-rich gas hydrates. This incident has highlighted the favorable effect of CO2 hydrate formation and needs to incorporate the chemo-processes into existing thermo-hydro-mechanical formulations. This paper presents an analytical formulation to capture the coupled thermo-hydro-chemo-mechanical behavior of gas hydrate-bearing sediments during gas production via CO2 injection. The key features of the formulation include hydrate formation and dissociation, gas dissolution and multiphase flow for both CH4 and CO2, facilitating CH4-CO2 hydrate conversion.
    Type: Book chapter , NonPeerReviewed
    DOI: 10.1061/9780784480137.024
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    OceanRep: Book chapter
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