Citation: | SUN Shicai, TIAN Wanxin, MENG Qingguo, BU Qingtao, WU Nengyou, HUANG Li. Effect of mineral type on the formation of natural gas hydrate[J]. Marine Geology & Quaternary Geology, 2025, 45(2): 215-224. doi: 10.16562/j.cnki.0256-1492.2024053001 |
The formation of natural gas hydrates in sediments is constrained by various factors, among which the physical and chemical properties of the sediments should not be overlooked. Based on the mineral composition of sediments in the South China Sea, the formation of natural gas hydrate was simulated experimentally by using four different minerals, olivine, carbonate, feldspar, and quartz. Results show that at low water saturation, the stronger hydrophilicity of the mineral, the longer the hydrate nucleation time; while at high water saturation, the effect of mineral hydrophilicity is weakened, the hydrate nucleation time is similar among the four minerals. The hydrate growth rate of olivine is the fastest, while quartz is the slowest. Additionally, the hydrate in all four minerals showed the characteristic of growing from sediment to the upper gas-phase space, which resulted in a trend of rapid growth followed by slow growth and then rapid growth of hydrates. The final hydrate saturation of the four minerals under same moisture content conditions was similar, ranging 12.52%~34.32%. The experimental results provide a reference for geological exploration and site selection for hydrate mining.
[1] | Malagar B R C, Lijith K P, Singh D N. Formation & dissociation of methane gas hydrates in sediments: a critical review[J]. Journal of Natural Gas Science and Engineering, 2019, 65:168-184. doi: 10.1016/j.jngse.2019.03.005 |
[2] | Sloan E D. Gas hydrates: review of physical/chemical properties[J]. Energy & Fuels, 1998, 12(2):191-196. |
[3] | Makogon Y F, Holditch S A, Makogon T Y. Natural gas-hydrates: a potential energy source for the 21st Century[J]. Journal of Petroleum Science and Engineering, 2007, 56(1-3):14-31. doi: 10.1016/j.petrol.2005.10.009 |
[4] | Misyura S Y. The influence of porosity and structural parameters on different kinds of gas hydrate dissociation[J]. Scientific Reports, 2016, 6:30324. doi: 10.1038/srep30324 |
[5] | Ren J J, Liu X H, Niu M Y, et al. Effect of sodium montmorillonite clay on the kinetics of CH4 hydrate-implication for energy recovery[J]. Chemical Engineering Journal, 2022, 437:135368. doi: 10.1016/j.cej.2022.135368 |
[6] | Chen C, Zhang Y, Li X S, et al. Investigations into methane hydrate formation, accumulation, and distribution in sediments with different contents of Illite clay[J]. Applied Energy, 2024, 359:122661. doi: 10.1016/j.apenergy.2024.122661 |
[7] | Mi F Y, He Z J, Zhao Y J, et al. Effects of surface property of mixed clays on methane hydrate formation in nanopores: a molecular dynamics study[J]. Journal of Colloid and Interface Science, 2022, 627:681-691. doi: 10.1016/j.jcis.2022.07.101 |
[8] | 孙始财, 业渝光, 刘昌岭, 等. 甲烷水合物在石英砂中生成过程研究[J]. 石油与天然气化工, 2011, 40(2):123-127 SUN Shicai. , YE Yuguang, LIU Changling, et al. Research of methane hydrate formation process in quartz sand[J]. Chemical Engineering of Oil and Gas, 2011, 40(2):123-127.] |
[9] | Babu P, Yee D, Linga P, et al. Morphology of methane hydrate formation in porous media[J]. Energy & Fuels, 2013, 27(6):3364-3372. |
[10] | Zhang B, Zhou L H, Liu C L, et al. Influence of sediment media with different particle sizes on the nucleation of gas hydrate[J]. Natural Gas Industry B, 2018, 5(6):652-659. doi: 10.1016/j.ngib.2018.11.001 |
[11] | Eswari C V V, Raju B, Chari V D, et al. Laboratory study of methane hydrate formation kinetics and structural stability in sediments[J]. Marine and Petroleum Geology, 2014, 58:199-205. doi: 10.1016/j.marpetgeo.2014.08.010 |
[12] | Maiti M, Bhaumik A K, Mandal A. Geological characterization of natural gas hydrate bearing sediments and their influence on hydrate formation and dissociation[J]. Journal of Natural Gas Science and Engineering, 2022, 100:104491. doi: 10.1016/j.jngse.2022.104491 |
[13] | Qin X W, Lu C, Wang P K, et al. Hydrate phase transition and seepage mechanism during natural gas hydrates production tests in the South China Sea: a review and prospect[J]. China Geology, 2022, 5(2):201-217. |
[14] | Sloan E D Jr, Koh C A. Clathrate Hydrates of Natural Gases[M]. 3rd ed. Boca Raton: CRC Press, 2007. |
[15] | Esmail S, Beltran J G. Methane hydrate propagation on surfaces of varying wettability[J]. Journal of Natural Gas Science and Engineering, 2016, 35:1535-1543. doi: 10.1016/j.jngse.2016.06.068 |
[16] | Qin Y, Shang L Y, Lv Z B, et al. Methane hydrate formation in porous media: overview and perspectives[J]. Journal of Energy Chemistry, 2022, 74:454-480. doi: 10.1016/j.jechem.2022.07.019 |
[17] | 张郁, 吴慧杰, 李小森, 等. 多孔介质中甲烷水合物的生成特性的实验研究[J]. 化学学报, 2011, 69(19):2221-2227 ZHANG Yu, WU Huijie, LI Xiaosen, et al. Experimental study on formation behavior of methane hydrate in porous media[J]. Acta Chimica Sinica, 2011, 69(19):2221-2227. |
[18] | Ke W, Svartaas T M, Chen D Y. A review of gas hydrate nucleation theories and growth models[J]. Journal of Natural Gas Science and Engineering, 2019, 61:169-196. doi: 10.1016/j.jngse.2018.10.021 |
[19] | Taylor C J, Miller K T, Koh C A, et al. Macroscopic investigation of hydrate film growth at the hydrocarbon/water interface[J]. Chemical Engineering Science, 2007, 62(23):6524-6533. doi: 10.1016/j.ces.2007.07.038 |
[20] | Chen Y, Gao Y H, Zhang N T, et al. Microfluidics application for monitoring hydrate phase transition in flow throats and evaluation of its saturation measurement[J]. Chemical Engineering Journal, 2020, 383:123081. doi: 10.1016/j.cej.2019.123081 |
[21] | Liang S, Kusalik P G. Explorations of gas hydrate crystal growth by molecular simulations[J]. Chemical Physics Letters, 2010, 494(4-6):123-133. doi: 10.1016/j.cplett.2010.05.088 |
[22] | 王亚东, 赵建忠, 高强, 等. 石英砂介质中甲烷水合物生成过程和相平衡的实验研究[J]. 石油与天然气化工, 2018, 47(6):44-49 doi: 10.3969/j.issn.1007-3426.2018.06.009 WANG Yadong, ZHAO Jianzhong, GAO Qiang, et al. Experimental study on the formation and phase equilibria of methane hydrate in quartz sand media[J]. Chemical Engineering of Oil and Gas, 2018, 47(6):44-49.] doi: 10.3969/j.issn.1007-3426.2018.06.009 |
[23] | Jin Y, Konno Y, Nagao J. Growth of methane clathrate hydrates in porous media[J]. Energy & Fuels, 2012, 26(4):2242-2247. |
[24] | Guo G J, Li M, Zhang Y G, et al. Why can water cages adsorb aqueous methane? A potential of mean force calculation on hydrate nucleation mechanisms[J]. Physical Chemistry Chemical Physics, 2009, 11(44):10427-10437. doi: 10.1039/b913898f |
The experimental setup for hydrate formation simulation
Sample density measurement
Comparison of nucleation time of hydrates in four minerals at different moisture contents
Changes in system temperature, pressure, and hydrate saturation during hydrate formation under the condition of 85% initial moisture content
Comparison of the growth time of hydrates in four minerals at different moisture contents
Hydrate growth in four sediment minerals at 70% initial moisture content
Changes in system temperature, pressure, and hydrate saturation during hydrate formation under the condition of 25% initial moisture content
Changes in system temperature, pressure, and hydrate saturation during hydrate formation under the condition of 40% initial moisture content
Changes in system temperature, pressure, and hydrate saturation during hydrate formation under the condition of 55% initial moisture content
Changes in system temperature, pressure, and hydrate saturation during hydrate formation under the condition of 70% initial moisture content