Methane Hydrate Formation and Dissociation in Sand Media: Effect of Water Saturation, Gas Flowrate and Particle Size
Abstract
:1. Introduction
2. Materials and Methods
2.1. Materials
2.2. Experimental Setup
2.3. Experimental Method
2.4. Study of Water Distribution by X-Ray Computerized Tomography (CT Scan)
3. Results
3.1. Water Distribution in Sandy Core Samples
- (1)
- Water injected at the top of the cell is heterogeneously distributed in the sandy core by capillary forces for 10% and 30% water saturation, in agreement with a previous finding [48]. Moreover, the amount of injected water is not sufficient to reach the bottom of the cell and a non-planar water front separating the wet and dry core sections is observed in Figure 5D. When the water saturation increases from 10% to 30%, this water front moves towards the bottom of the cell. The penetration depth of the water is between 4 cm and 6 cm thickness at 10% saturation, and between 8 cm and 10 cm thickness at 30%.
- (2)
- For higher water saturations (50% and 75%), the interface between the wet and dry core sections is not observed: it can be assumed that the amount of water is sufficient to reach the bottom of the cell. This is supported by the fact that the network cracks (J) reach the bottom of the cell at 50% water saturation. However, these CT scan images do not provide detailed and conclusive information on the total wettability of the core, and some zones remain dry suggesting a spatial heterogeneity as observed by Song et al. [49]. Therefore, Figure 5 should not be taken as face value but rather as an illustration of how heterogeneities linked to the intrinsic properties of the sandy particles (porosity and permeability) can be reflected in the water distribution. The computed porosity of the sandy core is around 0.42 here. Intrinsic permeability measurements were not carried out as our apparatus was not designed for this purpose. However, it was possible to calculate a first-order estimate of the hydraulic conductivity (k) using two widely used formula for coarse-grained matrices: The correlation from Hazen (1892) that correlated k with the effective diameter of the finest 10% of the sand (D10), and an analytically derived Kozeny-Carman’s equation from Ren et al. (2018) which is a function of the specific surface area of the sand [50,51,52,53,54]. The hydraulic conductivity is proportional to the intrinsic permeability, and gives an idea on how water flows through the sandy core. Here, computed hydraulic conductivity values are of (in cm·s−1) from 2 × 10−2 to 5 × 10−2, from 1 × 10−2 to 3 × 10−2 and from 6 × 10−2 to 17 × 10−2 for the non-sieved sand, and the fraction PS01 and PS03, respectively. The highest values are obtained with the correlation derived from Kozeny-Carman’s equation. As expected, the hydraulic conductivity increases with increasing particle size. These values are in agreement with values from the literature for sand with similar D10 [51,52,53]. Overall, there is less than one order of magnitude between the hydraulic conductivity of each sand fraction. Knowing the non-compressibility of sand particles, we can reasonably consider here a narrow distribution range for their intrinsic permeability of the core and a diversity in the flow paths due to differences in size and shape of the particles, thus, explaining the heterogeneity in the porosity and permeability fields. In fact, the non-planar waterfront after water stabilization at 10 and 30% water saturation results from heterogeneity in the porosity and permeability fields. Thus, it is likely that even if the same procedure for sample preparation is repeated with the same matrix and at the same water saturation, the water distribution may differ from one experiment to another. At 75% water saturation, we noticed the presence of a region with a cone-like shape located in the center of the core. This region corresponds to a water saturated zone as the water injection point is located at the center of the cell lid, this assumption was confirmed when emptying the cell to visually examine the sandy core. The small region with a cone-like shape of wet sand was indeed visible, and it took longer to defrost compared to the rest of the matrix.
3.2. Hydrate Formation: Variability of the Induction Time and Pressure Induced Growth Trajectory with the Three Selected Parameters
3.2.1. Evolution of Induction Time for Repeated Experiments
3.2.2. Influence of Water Saturation
3.2.3. Influence of Particle Size
3.2.4. Influence of the Gas Flowrate
3.3. Influence of the Water Conversion, Gas Injection Flowrate and Particle Size on the Storage Capacity
4. Conclusions
Supplementary Materials
Author Contributions
Funding
Acknowledgments
Conflicts of Interest
References
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Particle Class | Fontainebleau Sand | PS01 | PS03 |
---|---|---|---|
Particle size by sieving (µm) | 80–450 | 80–140 | 315–450 |
Particle size by diffractometer analysis (µm) | 80–450 | 80–200 | 200–550 |
Mass (g) | 100 | 5.8 | 4.2 |
Porous stone diameter (cm) | 5.54 ± 0.88 |
Aluminum cell internal diameter (cm) | 5.6 ± 0.01 |
Aluminum lids internal diameter (cm) | 0.57 ± 0.01 |
Porous stone depth (cm) | 0.6 ± 0.2 |
Aluminum cell height (cm) | 13.94 ± 0.01 |
Aluminum lids height (cm) | 5.55 ± 0.01 |
Sand density (g·cm−3) | 2.65 ± 0.01 |
Porosity | 0.42 ± 7.103 |
Run. | Water Volume (mL) | Water Saturation, Sw (%) | Gas Flowrate (mLn/min) | Particle Size (µm) | Induction Time (min) | Volume of Hydrate-Bound Methane (Ln) | Water Conversion (% vol) |
---|---|---|---|---|---|---|---|
1 | 23.34 | 10.8 | 56.1 | 80–450 | 53 | 4.94 | 97.8 |
2 | 46.6 | 21.6 | 58.5 | 65 | 8.27 | 82.0 | |
3 | 72.4 | 33 | 58.4 | 148 | 10.50 | 67.0 | |
4 | 92.69 | 44 | 57.6 | 63 | 15.82 | 78.9 | |
5_1 * | 116.5 | 53 | 57.5 | 82 | 15.48 | 61.4 | |
5_2 * | 116.1 | 54 | 58.8 | 57 | 12.44 | 49.5 | |
5_3 * | 117.3 | 54 | 57.2 | 55 | 14.77 | 58.2 | |
5_4 * | 117.8 | 55 | 57.9 | 51 | 20.94 | 82.1 | |
5_5 * | 124.8 | 57 | 57.5 | 47 | 20.43 | 75.6 | |
6 | 144.9 | 66.3 | 58.2 | 69 | 25.43 | 82.7 |
Gas Flowrate (mLn·min−1) | Water Volume (mL) | Water Saturation, Sw (%) | Particle Size Class (µm) | Induction Time (min) | Volume of Hydrate-Bound Methane (Ln) | Water Conversion (%) |
---|---|---|---|---|---|---|
56.8 | 129.0 | 54.3 | PS01 | 83 | 23.91 | 86.0 |
57.9 | 117.8 | 55.0 | non-sieved sand | 51 | 20.94 | 82.1 |
58.0 | 117.2 | 54.6 | PS03 | 52 | 21.83 | 86.1 |
28.9 | 125.9 | 53.7 | PS01 | 129.5 | 22.74 | 83.5 |
29.0 | 115.7 | 54.2 | non-sieved sand | 85 | 21.59 | 84.0 |
28.8 | 111.3 | 50.9 | PS03 | 109 | 17.81 | 74.0 |
86.5 | 125.7 | 53.3 | PS01 | 40.3 | 17.05 | 62.7 |
87.6 | 115.9 | 53.9 | PS03 | 30.3 | 21.29 | 84.9 |
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Benmesbah, F.D.; Ruffine, L.; Clain, P.; Osswald, V.; Fandino, O.; Fournaison, L.; Delahaye, A. Methane Hydrate Formation and Dissociation in Sand Media: Effect of Water Saturation, Gas Flowrate and Particle Size. Energies 2020, 13, 5200. https://doi.org/10.3390/en13195200
Benmesbah FD, Ruffine L, Clain P, Osswald V, Fandino O, Fournaison L, Delahaye A. Methane Hydrate Formation and Dissociation in Sand Media: Effect of Water Saturation, Gas Flowrate and Particle Size. Energies. 2020; 13(19):5200. https://doi.org/10.3390/en13195200
Chicago/Turabian StyleBenmesbah, Fatima Doria, Livio Ruffine, Pascal Clain, Véronique Osswald, Olivia Fandino, Laurence Fournaison, and Anthony Delahaye. 2020. "Methane Hydrate Formation and Dissociation in Sand Media: Effect of Water Saturation, Gas Flowrate and Particle Size" Energies 13, no. 19: 5200. https://doi.org/10.3390/en13195200