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Energies
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Carbon Dioxide Storage in Hydrate Reservoirs
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Carbon Dioxide Storage in Hydrate Reservoirs

A special issue of Energies (ISSN 1996-1073). This special issue belongs to the section "H: Geo-Energy".

Deadline for manuscript submissions: closed (25 February 2021) | Viewed by 11081

Special Issue Editor

Priv. Doz. Dr. Judith M. Schicks

E-Mail Website
Guest Editor
GFZ German Research Centre for Geosciences, Telegrafenberg, 14473 Potsdam, Germany
Interests: thermodynamic and kinetic aspects of natural gas hydrates; development and test of methods for the exploitation of natural gas hydrates; interactions between gas hydrates and microorganism; natural gas hydrate response to climate changes
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Emissions of anthropogenic carbon dioxide (CO2) into the atmosphere are widely accepted to be the main driver of climate change. The reduction of CO2 emissions, therefore, is a major aim for mitigation pathways, in order to minimize the effects of this greenhouse gas on the global climate. In recent decades, carbon capture and storage (CCS) has been discussed as a potential approach to reach this objective. The injection of CO2 into hydrate reservoirs is one potential alternative for the storage of CO2. Carbon dioxide storage in hydrate reservoirs is an ongoing discussion, involving possible opportunities, technical challenges, and potential risks. This Special Issue seeks to contribute to this discussion through enhanced scientific and multidiscipline studies in this research area. Topics of interest for publication include but are not limited to:

  • Interactions between the injected CO2 and the initial natural gas hydrate and the CO2 enclathration process on a molecular level;
  • Interactions between sediments, microorganisms, and the injected CO2, and their influence on the resulting hydrate phase;
  • Multiphase behavior of pore water, injected CO2, and the hydrate phase;
  • CO2 hydrate formation process and kinetics under conditions close to nature;
  • Evaluation of the economic feasibility of the usage of CO2 as a method for CH4 production from natural gas hydrate reservoirs;
  • Technical challenges and developments related to the storage of CO2 in natural gas hydrate reservoirs;
  • Predictions of the long-term behavior of injected CO2 in hydrates and sustainability of CO2 storage;
  • Assessment of potential environmental risks.

Publications based on field data, experimental, and/or modeling studies are highly welcome contributions to this Special Issue.

Priv. Doz. Dr. Judith M. Schicks
Guest Editor

Manuscript Submission Information

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Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2600 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • Gas hydrates
  • Thermodynamic behavior
  • Kinetics
  • CO2–CH4 replacement
  • Environmental impact of CO2 injection into hydrate reservoirs
  • Sustainability of CO2 storage in hydrates
  • Economic feasibility of CO2 storage in hydrates

Published Papers (4 papers)

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Research

31 pages, 7248 KiB  
Article
Microscale Processes and Dynamics during CH4–CO2 Guest-Molecule Exchange in Gas Hydrates
by Elke Kossel, Nikolaus K. Bigalke, Christian Deusner and Matthias Haeckel
Energies 2021, 14(6), 1763; https://doi.org/10.3390/en14061763 - 22 Mar 2021
Cited by 5 | Viewed by 1691
Abstract
The exchange of CH4 by CO2 in gas hydrates is of interest for the production of natural gas from methane hydrate with net zero climate gas balance, and for managing risks that are related to sediment destabilization and mobilization after gas-hydrate [...] Read more.
The exchange of CH4 by CO2 in gas hydrates is of interest for the production of natural gas from methane hydrate with net zero climate gas balance, and for managing risks that are related to sediment destabilization and mobilization after gas-hydrate dissociation. Several experimental studies on the dynamics and efficiency of the process exist, but the results seem to be partly inconsistent. We used confocal Raman spectroscopy to map an area of several tens to hundreds µm of a CH4 hydrate sample during its exposure to liquid and gaseous CO2. On this scale, we could identify and follow different processes in the sample that occur in parallel. Next to guest-molecule exchange, gas-hydrate dissociation also contributes to the release of CH4. During our examination period, about 50% of the CO2 was bound by exchange for CH4 molecules, while the other half was bound by new formation of CO2 hydrates. We evaluated single gas-hydrate grains with confirmed gas exchange and applied a diffusion equation to quantify the process. Obtained diffusion coefficients are in the range of 10−13–10−18 m2/s. We propose to use this analytical diffusion equation for a simple and robust modeling of CH4 production by guest-molecule exchange and to combine it with an additional term for gas-hydrate dissociation. Full article
(This article belongs to the Special Issue Carbon Dioxide Storage in Hydrate Reservoirs)
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23 pages, 4706 KiB  
Article
New Insights on a µm-Scale into the Transformation Process of CH4 Hydrates to CO2-Rich Mixed Hydrates
by Mengdi Pan, Nur Aminatulmimi Ismail, Manja Luzi-Helbing, Carolyn A. Koh and Judith M. Schicks
Energies 2020, 13(22), 5908; https://doi.org/10.3390/en13225908 - 12 Nov 2020
Cited by 9 | Viewed by 2105
Abstract
The global occurrences of natural gas hydrates lead to the conclusion that tremendous amounts of hydrocarbons are bonded in these hydrate-bearing sediments, serving as a potential energy resource. For the release of the hydrate-bonded CH4 from these reservoirs, different production methods have [...] Read more.
The global occurrences of natural gas hydrates lead to the conclusion that tremendous amounts of hydrocarbons are bonded in these hydrate-bearing sediments, serving as a potential energy resource. For the release of the hydrate-bonded CH4 from these reservoirs, different production methods have been developed during the last decades. Among them, the chemical stimulation via injection of CO2 is considered as carbon neutral on the basis of the assumption that the hydrate-bonded CH4 is replaced by CO2. For the investigation of the replacement process of hydrate-bonded CH4 with CO2 on a µm-scale, we performed time-resolved in situ Raman spectroscopic measurements combined with microscopic observations, exposing the CH4 hydrates to a CO2 gas phase at 3.2 MPa and 274 K. Single-point Raman measurements, line scans and Raman maps were taken from the hydrate phase. Measurements were performed continuously at defined depths from the surface into the core of several hydrate crystals. Additionally, the changes in composition in the gas phase were recorded. The results clearly indicated the incorporation of CO2 into the hydrate phase with a concentration gradient from the surface to the core of the hydrate particle, supporting the shrinking core model. Microscopic observations, however, indicated that all the crystals changed their surface morphology when exposed to the CO2 gas. Some crystals of the initial CH4 hydrate phase grew or were maintained while at the same time other crystals decreased in sizes and even disappeared over time. This observation suggested a reformation process similar to Ostwald ripening rather than an exchange of molecules in already existing hydrate structures. The experimental results from this work are presented and discussed in consideration of the existing models, providing new insights on a µm-scale into the transformation process of CH4 hydrates to CO2-rich mixed hydrates. Full article
(This article belongs to the Special Issue Carbon Dioxide Storage in Hydrate Reservoirs)
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13 pages, 4060 KiB  
Article
Hydrate Plugging and Flow Remediation during CO2 Injection in Sediments
by Jarand Gauteplass, Stian Almenningen, Tanja Barth and Geir Ersland
Energies 2020, 13(17), 4511; https://doi.org/10.3390/en13174511 - 01 Sep 2020
Cited by 21 | Viewed by 3473
Abstract
Successful geological sequestration of carbon depends strongly on reservoir seal integrity and storage capacity, including CO2 injection efficiency. Formation of solid hydrates in the near-wellbore area during CO2 injection can cause permeability impairment and, eventually, injectivity loss. In this study, flow [...] Read more.
Successful geological sequestration of carbon depends strongly on reservoir seal integrity and storage capacity, including CO2 injection efficiency. Formation of solid hydrates in the near-wellbore area during CO2 injection can cause permeability impairment and, eventually, injectivity loss. In this study, flow remediation in hydrate-plugged sandstone was assessed as function of hydrate morphology and saturation. CO2 and CH4 hydrates formed consistently at elevated pressures and low temperatures, reflecting gas-invaded zones containing residual brine near the injection well. Flow remediation by methanol injection benefited from miscibility with water; the methanol solution contacted and dissociated CO2 hydrates via liquid water channels. Injection of N2 gas did not result in flow remediation of non-porous CO2 and CH4 hydrates, likely due to insufficient gas permeability. In contrast, N2 as a thermodynamic inhibitor dissociated porous CH4 hydrates at lower hydrate saturations (<0.48 frac.). Core-scale thermal stimulation proved to be the most efficient remediation method for near-zero permeability conditions. However, once thermal stimulation ended and pure CO2 injection recommenced at hydrate-forming conditions, secondary hydrate formation occurred aggressively due to the memory effect. Field-specific remediation methods must be included in the well design to avoid key operational challenges during carbon injection and storage. Full article
(This article belongs to the Special Issue Carbon Dioxide Storage in Hydrate Reservoirs)
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17 pages, 2166 KiB  
Article
Analysis of the Dissolution of CH4/CO2-Mixtures into Liquid Water and the Subsequent Hydrate Formation via In Situ Raman Spectroscopy
by Zheng Li, Christine C. Holzammer and Andreas S. Braeuer
Energies 2020, 13(4), 793; https://doi.org/10.3390/en13040793 - 11 Feb 2020
Cited by 3 | Viewed by 3277
Abstract
We report an experimental study for the investigation into the suitability of hydrate formation processes for the purification of methane (CH4) from carbon dioxide (CO2) at a sub-cooling temperature of 6 K and a pressure of 4 MPa. The [...] Read more.
We report an experimental study for the investigation into the suitability of hydrate formation processes for the purification of methane (CH4) from carbon dioxide (CO2) at a sub-cooling temperature of 6 K and a pressure of 4 MPa. The experiments were conducted in a stirred batch reactor. Three different initial CH4/CO2 mixtures with methane fractions of 70.1 mol%, 50.3 mol%, and 28.5 mol% were tested. The separation efficiency was quantified by measuring in situ via Raman spectroscopy the ratios of CH4/CO2 in the gas mixture, the liquid water-rich phase before hydrate formation, and the solid hydrate phase after the onset of the hydrate formation. The results indicated that the main separation effect is obtained due to the preferential dissolution of CO2 into the liquid water-rich phase before the onset of the hydrate formation. Full article
(This article belongs to the Special Issue Carbon Dioxide Storage in Hydrate Reservoirs)
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