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Structural transition induced by cage-dependent guest exchange in CH4 + C3H8 hydrates with CO2 injection for energy recovery and CO2 sequestration

Author

Listed:
  • Lee, Yohan
  • Choi, Wonjung
  • Seo, Young-ju
  • Lee, Joo Yong
  • Lee, Jaehyoung
  • Seo, Yongwon

Abstract

This study investigated a structural transition induced by cage-dependent guest exchange in the CH4 + C3H8 hydrate with CO2 injection for CH4 recovery and CO2 sequestration. The influence of the CO2 replacement on the crystalline structure of initial CH4 + C3H8 hydrates and the cage-dependent distribution of guest molecules were quantitatively investigated using powder X-ray diffraction, 13C nuclear magnetic resonance spectroscopy, and gas chromatography. The quantitative analyses demonstrated that the CO2 occupation caused the depletion of C3H8 molecules in the large 51264 cages of structure II hydrates, thereby resulting in the subsequent transformation into CO2-rich sI hydrates and the coexistence of structure I and structure II hydrates after the replacement. The guest-exchange behavior observed from time-dependent Raman spectra indicated that the replacement rate was increased with an increase in pressure of injected CO2 and that the extent of the replacement was enhanced at higher pressure of injected CO2. Overall experimental evidence of the partial structural-transition replacement suggests that CO2 molecules first occupied structure II hydrates predominantly with the rapid guest exchange at the surface and that the initial structure II hydrates were subsequently converted to the CO2-rich structure I hydrates from the surface to the inner side. Precise identification of the mechanism responsible for the partial structural transition occurring in the CH4 + C3H8 - CO2 replacement will be very helpful in developing a strategy for actual CO2 injection into structure II gas hydrate reservoirs for energy recovery and CO2 sequestration.

Suggested Citation

  • Lee, Yohan & Choi, Wonjung & Seo, Young-ju & Lee, Joo Yong & Lee, Jaehyoung & Seo, Yongwon, 2018. "Structural transition induced by cage-dependent guest exchange in CH4 + C3H8 hydrates with CO2 injection for energy recovery and CO2 sequestration," Applied Energy, Elsevier, vol. 228(C), pages 229-239.
  • Handle: RePEc:eee:appene:v:228:y:2018:i:c:p:229-239
    DOI: 10.1016/j.apenergy.2018.06.088
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    References listed on IDEAS

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    Cited by:

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    4. Sun, You-Hong & Zhang, Guo-Biao & Carroll, John J. & Li, Sheng-Li & Jiang, Shu-Hui & Guo, Wei, 2018. "Experimental investigation into gas recovery from CH4-C2H6-C3H8 hydrates by CO2 replacement," Applied Energy, Elsevier, vol. 229(C), pages 625-636.
    5. Chun-Gang Xu & Min Wang & Gang Xu & Xiao-Sen Li & Wei Zhang & Jing Cai & Zhao-Yang Chen, 2021. "The Relationship between Thermal Characteristics and Microstructure/Composition of Carbon Dioxide Hydrate in the Presence of Cyclopentane," Energies, MDPI, vol. 14(4), pages 1-17, February.
    6. Choi, Wonjung & Lee, Yohan & Mok, Junghoon & Seo, Yongwon, 2020. "Influence of feed gas composition on structural transformation and guest exchange behaviors in sH hydrate – Flue gas replacement for energy recovery and CO2 sequestration," Energy, Elsevier, vol. 207(C).
    7. Mok, Junghoon & Choi, Wonjung & Seo, Yongwon, 2021. "The dual-functional roles of N2 gas for the exploitation of natural gas hydrates: An inhibitor for dissociation and an external guest for replacement," Energy, Elsevier, vol. 232(C).
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    9. Zhong, Jin-Rong & Sun, Yi-Fei & Li, Wen-Zhi & Xie, Yan & Chen, Guang-Jin & Sun, Chang-Yu & Yang, Lan-Ying & Qin, Hui-Bo & Pang, Wei-Xin & Li, Qing-Ping, 2019. "Structural transition range of methane-ethane gas hydrates during decomposition below ice point," Applied Energy, Elsevier, vol. 250(C), pages 873-881.
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