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Isostructural and cage-specific replacement occurring in sII hydrate with external CO2/N2 gas and its implications for natural gas production and CO2 storage

Author

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  • Seo, Young-ju
  • Park, Seongmin
  • Kang, Hyery
  • Ahn, Yun-Ho
  • Lim, Dongwook
  • Kim, Se-Joon
  • Lee, Jaehyoung
  • Lee, Joo Yong
  • Ahn, Taewoong
  • Seo, Yongwon
  • Lee, Huen

Abstract

A replacement technique has been regarded as a promising strategy for both CH4 exploitation from gas hydrates and CO2 sequestration into deep-ocean reservoirs. Most research has been focused on replacement reactions that occur in sI hydrates due to their prevalence in natural gas hydrates. However, sII hydrates in nature have been also discovered in some regions, and the replacement mechanism in sII hydrates significantly differs from that in sI hydrates. In this study, we have intensively investigated the replacement reaction of sII (C3H8+CH4) hydrate by externally injecting CO2/N2 (50:50) gas mixture with a primary focus on powder X-ray diffraction, Raman spectroscopy, NMR spectroscopy, and gas chromatography analyses. In particular, it was firstly confirmed that there was no structural transformation during the replacement of C3H8+CH4 hydrate with CO2/N2 gas injection, indicating that sII hydrate decomposition followed by sI hydrate formation did not occur. Furthermore, the cage-specific replacement pattern of the C3H8+CH4 hydrate revealed that CH4 replacement with N2 in the small cages of sII was more significant than C3H8 replacement with CO2 in the large cages of sII. The total extent of the replacement for the C3H8+CH4 hydrate was cross-checked by NMR and GC analyses and found to be approximately 54%. Compared to the replacement for CH4 hydrate with CO2/N2 gas, the lower extent of the replacement for the C3H8+CH4 hydrate with CO2/N2 gas was attributable to the persistent presence of C3H8 in the large cages and the lower content of N2 in the feed gas. The structural sustainability and cage-specific replacement observed in the C3H8+CH4 hydrate with external CO2/N2 gas will have significant implications for suggesting target gas hydrate reservoirs and understanding the precise nature of guest exchange in gas hydrates for both safe natural gas production and long-term CO2 sequestration.

Suggested Citation

  • Seo, Young-ju & Park, Seongmin & Kang, Hyery & Ahn, Yun-Ho & Lim, Dongwook & Kim, Se-Joon & Lee, Jaehyoung & Lee, Joo Yong & Ahn, Taewoong & Seo, Yongwon & Lee, Huen, 2016. "Isostructural and cage-specific replacement occurring in sII hydrate with external CO2/N2 gas and its implications for natural gas production and CO2 storage," Applied Energy, Elsevier, vol. 178(C), pages 579-586.
    • Handle: RePEc:eee:appene:v:178:y:2016:i:c:p:579-586
    DOI: 10.1016/j.apenergy.2016.06.072
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    6. Zang, Xiaoya & Zhou, Xuebing & Wan, Lihua & Wang, Jing & Liang, Deqing, 2020. "Investigation of hydrate formation by synthetic ternary gas mixture with cyclopentane(C5H10)," Energy, Elsevier, vol. 210(C).
    7. Song, Chunfeng & Liu, Qingling & Ji, Na & Deng, Shuai & Zhao, Jun & Kitamura, Yutaka, 2017. "Natural gas purification by heat pump assisted MEA absorption process," Applied Energy, Elsevier, vol. 204(C), pages 353-361.
    8. 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.
    9. 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.
    10. Chen, Ye & Gao, Yonghai & Zhao, Yipeng & Chen, Litao & Dong, Changyin & Sun, Baojiang, 2018. "Experimental investigation of different factors influencing the replacement efficiency of CO2 for methane hydrate," Applied Energy, Elsevier, vol. 228(C), pages 309-316.
    11. 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).
    12. Wang, Xiao-Hui & Sun, Yi-Fei & Wang, Yun-Fei & Li, Nan & Sun, Chang-Yu & Chen, Guang-Jin & Liu, Bei & Yang, Lan-Ying, 2017. "Gas production from hydrates by CH4-CO2/H2 replacement," Applied Energy, Elsevier, vol. 188(C), pages 305-314.
    13. Zang, Xiaoya & Wang, Jing & He, Yong & Zhou, Xuebing & Liang, Deqing, 2022. "Experimental investigation of hydrate formation kinetics and microscopic properties by a synthesized ternary gas mixture with combination additives," Energy, Elsevier, vol. 259(C).
    14. Tupsakhare, Swanand S. & Castaldi, Marco J., 2019. "Efficiency enhancements in methane recovery from natural gas hydrates using injection of CO2/N2 gas mixture simulating in-situ combustion," Applied Energy, Elsevier, vol. 236(C), pages 825-836.

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