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
Abstract
:1. Introduction
2. Experiments
2.1. Experimental Setups
2.2. Materials
2.3. Experimental Procedures
3. Results and Discussion
3.1. Phase Equilibrium of Mixed Gas Hydrates
3.2. CH4-CO2 Exchange between a Vapor Phase and a Bulk Gas Hydrate Phase
4. Conclusions
Author Contributions
Funding
Conflicts of Interest
Abbreviations
Term | Symbol | Unit |
Vapor phase composition of molecule i | yi | mole fraction |
Vapor phase composition of molecule i without H2O | y*i | mole fraction |
Gas hydrate composition of molecule i (i.e., hydration number for H2O) | hi | mole fraction |
Gas hydrate composition of guest molecule i | h*i | mole fraction |
Global composition of molecule i in the system | zi | mole fraction |
Global composition of molecule i in the system without H2O | z*i | mole fraction |
Appendix A
Time after Gas Replacement/h | T/K | p/MPa | y*CH4 Mole Fraction |
---|---|---|---|
0.53 | 277.0 | 3.38 | 0.049 |
0.97 | 277.8 | 3.45 | 0.178 |
1.47 | 277.8 | 3.39 | 0.318 |
2.65 | 277.8 | 3.22 | 0.368 |
18.90 | 277.7 | 2.78 | 0.530 |
89.73 | 277.7 | 2.85 | 0.586 |
118.90 | 277.8 | 2.88 | 0.597 |
145.73 | 277.7 | 2.90 | 0.603 |
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Reference | T/K p/MPa | CO2 Mole Fraction | Number of Data Points |
---|---|---|---|
[26] | 273.1–280.2 1.22–3.09 | z*CO2= 0.9099–0.9652 | 9 |
[27] | 273.4–281.9 1.986–9.550 | z*CO2 = 0.20–0.75 y*CO2 = 0.1620–0.7189 | 15 |
[28,29] | 272.85–284.25 1.565–24.12 | z*CO2 = 0.0663–0.9659 | 28 |
[30] | 273.7 7.7 | z*CO2 = 0.169 y*CO2 = 0.139 | 1 |
[31] | 275.3–283.1 1.6–22.4 | z*CO2 = 0.21–0.80 y*CO2 = 0.162–0.787 | 24 |
[32] | 273.4–281.1 5.30–6.60 | y*CO2 = 0.16–0.59 | 16 |
[33] | 276.88–285.41 5.0–20.0 | z*CO2 = 0.841–0.906 | 16 |
[34] | 273.6–281.7 2.032–17.628 | yCO2 = 0.127–0.747 | 35 |
[35] | 278.1–285.3 3.24–29.92 | z*CO2 = 0.271–0.812 | 9 |
[36] | 275.0–281.1 8.23–24.51 | z*CO2 = 0.1–0.2 | 17 |
[37] | 273.4–278.4 5.28–17.53 | z*CO2 = 0.101–0.251 | 17 |
[38] | 275.75–284.45 5–20 | z*CO2 = 0.26–0.36 | 10 |
[39] | 270.5–278.3 | z*CO2= 0.01–0.47 | 9 |
This work | 276.06–280.97 9.762–20.583 | z*CO2 = 0.2317 | 4 |
Reference | T/K p/MPa | CH4 Mole Fraction | CO2 Mole Fraction | N2 Mole Fraction | Number of Data Points |
---|---|---|---|---|---|
[40] | 276.85–293.41 3.454–23.979 | z*CH4 = 0.9497 | z*CO2 = 0.05 | z*N2 = 0.0003 | 6 |
[41] | ca. 274–282 ca. 2–5 | z*CH4 = 0.41–0.55 | z*CO2 = 0.29–0.40 | z*N2 = 0.05–0.30 | 26 |
[42] | 284.50–289.34 8.75–11.23 | z*CH4 = 0.8989 | z*CO2 = 0.05 | z*N2 = 0.0511 | 6 |
[43] | 279.6–293.0 4.81–30.66 | z*CH4 = 0.5–0.9 | z*CO2 = 0.02–0.1 | z*N2 = 0.08–0.4 | 30 |
[23] | 274.9–283.9 2.29–14.97 | y*CH4 = 0.203–0.826 | y*CO2 = 0.052–0.604 | y*N2 = 0.05–0.577 | 45 |
[44] | 276.2–286.3 2.59–8.84 | z*CH4 = 0.4995–0.7005 | z*CO2 = 0.1998–0.4503 | z*N2 = 0.0490–0.1093 | 34 |
This work | 282.46–288.62 9.679–15.645 | z*CH4 = 0.46–0.941 | z*CO2 = 0.015–0.14 | z*N2 = 0.044–0.379 | 5 |
T/K | p /Mpa Experiment | p/MPa CSMGem (Deviation %) [1] | z*N2 | z*CO2 | z*CH4 | H2O:Gas Feed Molar Ratio | H2O Saturation vol.% |
---|---|---|---|---|---|---|---|
276.06 | 9.762 | 11.165 (14.4) | 0.7683 | 0.2317 | 0 | 19.45 | 58.3 |
277.63 | 12.584 | 14.504 (15.3) | 0.7683 | 0.2317 | 0 | 21.52 | 66.8 |
279.09 | 16.373 | 18.539 (13.2) | 0.7683 | 0.2317 | 0 | 24.32 | 74.9 |
280.97 | 20.583 | 23.873 (16.0) | 0.7683 | 0.2317 | 0 | 24.25 | 78.2 |
280.92 | 3.410 | 3.5798 (5.0) | 0 | 0.8996 | 0.1004 | 44.66 | 83.2 |
282.61 | 4.291 | 4.3982 (2.5) | 0 | 0.8996 | 0.1004 | 37.46 | 83.2 |
284.97 | 6.206 | 6.3211 (1.9) | 0 | 0.8996 | 0.1004 | 42.47 | 91.9 |
282.46 | 9.679 | No convergence | 0.40 | 0.14 | 0.46 | 5.31 | 41.5 |
283.37 | 10.964 | 10.419 (−5.0) | 0.38 | 0.14 | 0.48 | 6.32 | 39.4 |
284.11 | 13.102 | 10.901 (−16.8) | 0.34 | 0.12 | 0.54 | 5.49 | 40.3 |
285.70 | 15.055 | 13.860 (−7.9) | 0.37 | 0.13 | 0.50 | 4.67 | 39.6 |
288.62 | 15.645 | 14.068 (−10.1) | 0.044 | 0.015 | 0.941 | 3.90 | 38.4 |
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Legoix, L.N.; Ruffine, L.; Deusner, C.; Haeckel, M. 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. Energies 2018, 11, 1984. https://doi.org/10.3390/en11081984
Legoix LN, Ruffine L, Deusner C, Haeckel M. 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. Energies. 2018; 11(8):1984. https://doi.org/10.3390/en11081984
Chicago/Turabian StyleLegoix, Ludovic Nicolas, Livio Ruffine, Christian Deusner, and Matthias Haeckel. 2018. "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" Energies 11, no. 8: 1984. https://doi.org/10.3390/en11081984