Journal of Petroleum Research

Journal of Petroleum Research

Experimental Study of Methane Hydrate Formation in Silica Porous Medium

Document Type : Research Paper

Authors
1 Institute of Petroleum Engineering, School of Chemical Engineering, College of Engineering, University of Tehran, IRAN
2 department of petroleum engineering, kish international campus, University of Tehran
3 School of Chemical Engineering, University of Tehran
DOI:10.22078/pr.2025.5733.3548
Abstract
Achieving methane production from a gas hydrate-containing system under safe and economic conditions requires a fundamental understanding of the physical behavior involved in the dynamic process of methane hydrate formation and separation in sedimentary environments. In this study, by designing a laboratory device, the kinetics of methane hydrate formation in a porous silica environment with an excess water approach in offshore fields were simulated. Also, using volume balance calculations, the methane conversion fraction during different stages of hydrate formation and the saturation of phases in hydrate-containing sediments were obtained. The results of the temperature and pressure evolution diagrams during the methane hydrate formation process showed that the hydrate formation conditions for laboratory samples are in great agreement with the prevailing thermodynamic conditions. In proportion to the selected silica sand grain size, the average saturation of the hydrate phase was 32.5%, the saturation of the water phase was 63.9%, and the saturation of the gas phase was 3.6% for laboratory samples. Furthermore, the average methane to hydrate conversion fraction for test samples was 88.2%. Moreover, the difference in the thermal responses of the system at some positions of the thermocouples was attributed to the non-uniform distribution and formation of methane hydrate in the porous medium. Also, the studies showed that the amount of access of gas and water phases and the type of distribution of the hydrate phase in the sedimentary medium are important factors controlling the methane conversion fraction in the experimental samples. The simulation of the temperature and pressure conditions of the gas hydrate formed in this study also had a good agreement with gas hydrate reservoirs in offshore fields.
Keywords

[1]. IEA (2019), World Energy Outlook; Paris.
[2]. Boswell, R., & Collett, T. S. (2011). Current perspectives on gas hydrate resources. Energy & environmental science, 4(4), 1206-1215.
[3]. Jarrahian, A., & Nakhaee, A. (2019). Hydrate–liquid–vapor equilibrium condition of N2+ CO2+ H2O system: Measurement and modeling. Fuel, 237, 769-774. doi.org/10.1016/j.fuel.2018.10.017.
[4]. Makogon YF(1997) Hydrates of hydrocarbons. Tulsa, Oklahoma: Pennwell Publishing Company.
[5]. Li, G., Moridis, G. J., Zhang, K., & Li, X. S. (2010). Evaluation of gas production potential from marine gas hydrate deposits in Shenhu area of South China Sea. Energy & Fuels, 24(11), 6018-6033.## doi.org/10.1021/ef100930m.
[6]. Moridis, G. J., Kowalsky, M. B., & Pruess, K. (2007). Depressurization-induced gas production from class 1 hydrate deposits. SPE Reservoir Evaluation & Engineering, 10(05), 458-481.
[7]. Moridis, G., & Collett, T. (2003). Strategies for gas production from hydrate accumulations under various geologic conditions.
[8]. Fujii, T., Saeki, T., Kobayashi, T., Inamori, T., Hayashi, M., Takano, O., Takayama, T., Kawasaki, T., Nagakubo, S., Nakamizu, M. and Yokoi, K., (2008). May. Resource assessment of methane hydrate in the eastern Nankai Trough, Japan. In Offshore technology conference (pp. OTC-19310). OTC. doi.org/10.4043/19310-MS.
[9]. Boswell R (2009). Is gas hydrate energy within reach? Science ;325:957.
[10]. Chong, Z. R., Yang, S. H. B., Babu, P., Linga, P., & Li, X. S. (2016). Review of natural gas hydrates as an energy resource: Prospects and challenges. Applied Energy, 162, 1633-1652. doi.org/10.1016/j.apenergy.2014.12.061.
[11]. Yin, Z., Chong, Z. R., Tan, H. K., & Linga, P. (2016). Review of gas hydrate dissociation kinetic models for energy recovery. Journal of Natural Gas Science and Engineering, 35, 1362-1387. doi: 10.1016/j.jngse.2016.04.050. 
[12]. Moridis, G.J., Collett, T.S., Pooladi-Darvish, M., Hancock, S., Santamarina, C., Boswell, R., Kneafsey, T., Rutqvist, J., Kowalsky, M.B., Reagan, M.T. and Sloan, E.D., 2011. Challenges, uncertainties, and issues facing gas production from gas-hydrate deposits. SPE reservoir evaluation & engineering, 14(01), pp.76-112. doi.org/10.2118/131792-PA.
[13]. Kneafsey, T. J., Tomutsa, L., Moridis, G. J., Seol, Y., Freifeld, B. M., Taylor, C. E., & Gupta, A. (2007). Methane hydrate formation and dissociation in a partially saturated core-scale sand sample. Journal of Petroleum Science and Engineering, 56(1-3), 108-126. doi: 10.1016/j.petrol.2006.02.002.
[14]. Liu, C., Lu, H., Ye, Y., Ripmeester, J. A., & Zhang, X. (2008). Raman spectroscopic observations on the structural characteristics and dissociation behavior of methane hydrate synthesized in silica sands with various sizes. Energy & fuels, 22(6), 3986-3988. doi.org/10.1021/ef800440s.
[15]. Zhou, Y., Castaldi, M. J., & Yegulalp, T. M. (2009). Experimental investigation of methane gas production from methane hydrate. Industrial & Engineering Chemistry Research, 48(6), 3142-3149. doi.org/10.1021/ie801004z.
[16]. Chong, Z. R., Pujar, G. A., Yang, M., & Linga, P. (2016). Methane hydrate formation in excess water simulating marine locations and the impact of thermal stimulation on energy recovery. Applied Energy, 177, 409-421. doi.org/10.1016/j.apenergy.2016.05.077.
[17]. Chong, Z. R., Zhao, J., Chan, J. H. R., Yin, Z., & Linga, P. (2018). Effect of horizontal wellbore on the production behavior from marine hydrate bearing sediment. Applied Energy, 214, 117-130. doi.org/10.1016/j.apenergy.2018.01.072.
[18]. Haligva, C., Linga, P., Ripmeester, J. A., & Englezos, P. (2010). Recovery of methane from a variable-volume bed of silica sand/hydrate by depressurization. Energy & Fuels, 24(5), 2947-2955. doi.org/10.1021/ef901220m.
[19]. Ruffine, L. (2015). Exploring methane-hydrate formation and dissociation in geologic materials through laboratory experiments: Kinetic behavior and morphology. Fuel, 141, 173-184. doi.org/10.1016/j.fuel.2014.10.041.
[20]. Li, B., Li, X. S., Li, G., Wang, Y., & Feng, J. C. (2014). Kinetic behaviors of methane hydrate formation in porous media in different hydrate deposits. Industrial & Engineering Chemistry Research, 53(13), 5464-5474. doi.org/10.1021/ie500580y.
[21]. Priest, J. A., Rees, E. V., & Clayton, C. R. (2009). Influence of gas hydrate morphology on the seismic velocities of sands. Journal of geophysical research: solid earth, 114(B11). doi.org/10.1029/2009JB006284.#
[22]. Spangenberg, E., Priegnitz, M., Heeschen, K. Gorelick S., & Schicks, J. M. (2015). Are laboratory-formed hydrate-bearing systems analogous to those in nature?. Journal of Chemical & Engineering Data, 60(2), 258-268. doi.org/10.1021/je5005609.
[23]. Choi, J. H., Dai, S., Cha, J. H., Gorelick S. & Seol, Y. (2014). Laboratory formation of noncementing hydrates in sandy sediments. Geochemistry, Geophysics, Geosystems, 15(4), 1648-1656. doi.org/10.1002/2014GC005287.
[24]. Chong, Z. R., Yin, Z., Gorelick S., Tan, J. H. C., & Linga, P. (2017). Experimental investigations on energy recovery from water-saturated hydrate bearing sediments via depressurization approach. Applied Energy, 204, 1513-1525. doi.org/10.1016/j.apenergy.2017.04.031.
[25] Razavizadeh, S. S., & Nakhaee, A. (2025). Experimental and modeling investigation of gas hydrate phase equilibrium for methane/propane/n-heptane (MPH) ternary hydrates. Geoenergy Science and Engineering, 247, 213690. doi: 10.1016/j.geoen.2025.213690.
[26] Makvandi, M., & Nakhaee, A. (2025). Investigating the Effect of Sodium Chloride on Methane Hydrate Equilibrium Conditions: Case Study of Caspian Sea Water Composition. Journal of Chemical and Petroleum Engineering, 59(1), 159-171. doi: 10.22059/jchpe.2024.382100.1559.
[27]. Schicks, J. M. (2022). Gas hydrates in nature and in the laboratory: necessary requirements for formation and properties of the resulting hydrate phase, department of geochemistry, GFZ German Research Centre for Geosciences, Telegrafenberg, 14473 Potsdam, Germany, Geoscience of Germany, ChemTexts, 8(2), 1-13. https://doi.org/10.1007/s40828-022-00164-3.#
[28]. Yin, Z., Huang, L., & Linga, P. (2019). Effect of wellbore design on the production behaviour of methane hydrate-bearing sediments induced by depressurization. Applied Energy, 254, 113635. doi.org/10.1016/j.apenergy.2019.113635.
[29]. Yin, Z., Wan, Q. C., Gao, Q., & Linga, P. (2020). Effect of pressure drawdown rate on the fluid production behaviour from methane hydrate-bearing sediments. Applied energy, 271, 115195. doi.org/10.1016/j.apenergy.2020.115195.
[30]. Mansouri, F. S., & Zui, V. I. (2019). Geothermal field and geology of the Caspian Sea region. Журнал Белорусского государственного университета. География. Геология, (1), 104-118.