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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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    Methane Production from Gas Hydrate Deposits through Injection of Supercritical CO2 (2012)
    MDPI
    In:  Energies, 5 (7). pp. 2112-2140.
    Details
    Publication Date: 2019-01-15
    Description: The recovery of natural gas from CH4-hydrate deposits in sub-marine and sub-permafrost environments through injection of CO2 is considered a suitable strategy towards emission-neutral energy production. This study shows that the injection of hot, supercritical CO2 is particularly promising. The addition of heat triggers the dissociation of CH4-hydrate while the CO2, once thermally equilibrated, reacts with the pore water and is retained in the reservoir as immobile CO2-hydrate. Furthermore, optimal reservoir conditions of pressure and temperature are constrained. Experiments were conducted in a high-pressure flow-through reactor at different sediment temperatures (2 °C, 8 °C, 10 °C) and hydrostatic pressures (8 MPa, 13 MPa). The efficiency of both, CH4 production and CO2 retention is best at 8 °C, 13 MPa. Here, both CO2- and CH4-hydrate as well as mixed hydrates can form. At 2 °C, the production process was less effective due to congestion of transport pathways through the sediment by rapidly forming CO2-hydrate. In contrast, at 10 °C CH4 production suffered from local increases in permeability and fast breakthrough of the injection fluid, thereby confining the accessibility to the CH4 pool to only the most prominent fluid channels. Mass and volume balancing of the collected gas and fluid stream identified gas mobilization as equally important process parameter in addition to the rates of methane hydrate dissociation and hydrate conversion. Thus, the combination of heat supply and CO2 injection in one supercritical phase helps to overcome the mass transfer limitations usually observed in experiments with cold liquid or gaseous CO2.
    Type: Article , PeerReviewed
    Format: text
    DOI: 10.3390/en5072112
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    OceanRep: Article in a Scientific Journal - peer-reviewed
  • 4
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    The Global Inventory of Methane Hydrate in Marine Sediments: A Theoretical Approach (2012)
    MDPI
    In:  Energies, 5 (7). pp. 2449-2498.
    Details
    Publication Date: 2019-09-23
    Description: The accumulation of methane hydrate in marine sediments is controlled by a number of physical and biogeochemical parameters including the thickness of the gas hydrate stability zone (GHSZ), the solubility of methane in pore fluids, the accumulation of particulate organic carbon at the seafloor, the kinetics of microbial organic matter degradation and methane generation in marine sediments, sediment compaction and the ascent of deep-seated pore fluids and methane gas into the GHSZ. Our present knowledge on these controlling factors is discussed and new estimates of global sediment and methane fluxes are provided applying a transport-reaction model at global scale. The modeling and the data evaluation yield improved and better constrained estimates of the global pore volume within the modern GHSZ ( ≥ 44 × 1015 m3), the Holocene POC accumulation rate at the seabed (~1.4 × 1014 g yr−1), the global rate of microbial methane production in the deep biosphere (4−25 × 1012 g C yr−1) and the inventory of methane hydrates in marine sediments ( ≥ 455 Gt of methane-bound carbon).
    Type: Article , PeerReviewed
    Format: text
    DOI: 10.3390/en5072449
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    OceanRep: Article in a Scientific Journal - peer-reviewed
  • 5
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    CO2 injection into submarine sediments: disturbing news for methane-rich hydrates (2011)
    HWU
    In:  [Poster] In: 7. International Conference on Gas Hydrates (ICGH 2011), 17.-21.07.2011, Edinburgh, Scotland, United Kingdom . Proceedings of the 7th International Conference on Gas Hydrates (ICGH2011) ; 591/1-9 .
    Details
    Publication Date: 2012-03-16
    Description: The production of natural gas via injection of fossil-fuel derived CO2 into submarine gas hydrate reservoirs can be an example of tapping a hydrocarbon energy source in a CO2-neutral manner. However, the industrial application of this method is technically challenging. Thus, prior to feasibility testing in the field, multi-scale laboratory experiments and adapted reaction-modeling are needed. To this end, high-pressure flow-through reactors of 15 and 2000 mL sample volume were constructed and tested. Process parameters (P, T, Q, fluid composition) are defined by a fluid supply and conditioning unit to enable simulation of natural fluid-flow scenarios for a broad range of sedimentary settings. Additional Raman- and NMR-spectroscopy aid in identifying the most efficient pathway for CH4 extraction from hydrates via CO2 injection on both microscopic and macroscopic level. In this study we present experimental set-up and design of the highpressure flow-through reactors as well as CH4 yields from H4-hydrate decomposition experiments using CO2-rich brines and pure liquefied CO2.
    Type: Conference or Workshop Item , NonPeerReviewed
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    OceanRep: Poster
  • 6
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    Report on range of long-term scenarios to be simulated (2012)
    ECO2 Project Office
    In:  ECO2 Deliverable, D12.2 . ECO2 Project Office, 6 pp.
    Details
    Publication Date: 2019-03-11
    Description: In order to proceed with speculative modelling of the impacts of potential leakage of geologically stored carbon, it is necessary to develop plausible scenarios. Here a range of such scenarios are developed based on a consensus of the possible geological mechanisms of leakage, namely abandoned wells, geological faults and operational blowouts. Whilst the resulting scenarios remain highly speculative, they do enable short term progress in modelling and provide a basis for further debate and refinement.
    Type: Report , NonPeerReviewed , info:eu-repo/semantics/book
    Format: text
    DOI: 10.3289/ECO2_D12.2
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    OceanRep: Report - other report
  • 7
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    CCT2 Report on model interfacing and evaluation strategy (2012)
    ECO2 Project Office
    In:  ECO2 Deliverable, D12.1 . ECO2 Project Office, 14 pp.
    Details
    Publication Date: 2019-03-11
    Type: Report , NonPeerReviewed , info:eu-repo/semantics/book
    Format: text
    DOI: 10.3289/ECO2_D12.1
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    OceanRep: Report - other report
  • 8
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    Report summarizing all information from WP2 relevant for the creation of an Environmental Best Practice for offshore CCS sites (2014)
    ECO2 Project Office
    In:  ECO2 Deliverable, D2.3 . ECO2 Project Office, Kiel, Germany, 13 pp.
    Details
    Publication Date: 2019-03-11
    Type: Report , NonPeerReviewed , info:eu-repo/semantics/book
    Format: text
    DOI: 10.3289/ECO2_D2.3
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    OceanRep: Report - other report
  • 9
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    Best Practice Guidance for Environmental Risk Assessment for offshore CO2 geological storage (2015)
    ECO2 Project Office
    In:  ECO2 Deliverable, D14.1 . ECO2 Project Office, Kiel, Germany, 53 pp.
    Details
    Publication Date: 2019-03-11
    Type: Report , NonPeerReviewed , info:eu-repo/semantics/book
    Format: text
    DOI: 10.3289/ECO2_D14.1
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    OceanRep: Report - other report
  • 10
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    3-D numerical modeling of methane hydrate deposits (2011)
    HWU
    In:  In: Proceedings of the 7th International Conference on Gas Hydrates (ICGH2011). HWU, Edinburgh, 279/1-6.
    Details
    Publication Date: 2012-07-06
    Description: Within the German gas hydrate initiative SUGAR, we have developed a new tool for predicting the formation of sub-seafloor gas hydrate deposits. For this purpose, a new 2D/3D module simulating the biogenic generation of methane from organic material and the formation of gas hydrates has been added to the petroleum systems modeling software package PetroMod®. T ypically, PetroMod® simulates the thermogenic generation of multiple hydrocarbon components including oil and gas, their migration through geological strata, and finally predicts the oil and gas accumulation in suitable reservoir formations. We have extended PetroMod® to simulate gas hydrate accumulations in marine and permafrost environments by the implementation of algorithms describing (1) the physical, thermodynamic, and kinetic properties of gas hydrates; and (2) a kinetic continuum model for the microbially mediated, low temperature degradation of particulate organic carbon in sediments. Additionally, the temporal and spatial resolutions of PetroMod® were increased in order to simulate processes on time scales of hundreds of years and within decimeters of spatial extension. As a first test case for validating and improving the abilities of the new hydrate module, the petroleum systems model of the Alaska North Slope developed by IES (currently Shlumberger) and the USGS has been chosen. In this area, gas hydrates have been drilled in several wells, and a field test for hydrate production is planned for 2011/2012. The results of the simulation runs in PetroMod® predicting the thickness of the gas hydrate stability field, the generation and migration of biogenic and thermogenic methane gas, and its accumulation as gas hydrates will be shown during the conference. The predicted distribution of gas hydrates will be discussed in comparison to recent gas hydrate findings in the Alaska North Slope region.
    Type: Book chapter , NonPeerReviewed
    Format: text
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    OceanRep: Book chapter
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