Microscopic experimental study on the effects of NaCl concentration on the self-preservation effect of methane hydrates under 268.15 K

doi:10.1016/j.cjche.2024.04.022

中国化学工程学报 ›› 2024, Vol. 73 ›› Issue (9): 1-14.DOI: 10.1016/j.cjche.2024.04.022

Microscopic experimental study on the effects of NaCl concentration on the self-preservation effect of methane hydrates under 268.15 K

Yu-Jie Zhu¹, Yu-Zhou Chen¹, Yan Xie², Jin-Rong Zhong³, Xiao-Hui Wang¹, Peng Xiao¹, Yi-Fei Sun¹, Chang-Yu Sun¹, Guang-Jin Chen¹

1. State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing 102249, China;
2. Research Centre of Ecology &Environment for Coastal Area and Deep Sea, Guangdong University of Technology, Guangzhou 510006, China;
3. School of Chemistry and Food Engineering, Changsha University of Science and Technology, Changsha 410114, China

收稿日期:2023-12-22 修回日期:2024-04-10 接受日期:2024-04-15 出版日期:2024-11-21 发布日期:2024-05-28
通讯作者: Xiao-Hui Wang,E-mail:xh.wang@cup.edu.cn;Chang-Yu Sun,E-mail:cysun@cup.edu.cn
基金资助:
The financial support received from the Basic Research Program of Qinghai Province (2023-ZJ-703), the National Natural Science Foundation of China (22178379, 42206223), and the National Key Research and Development Program of China (2021YFC2800902) is gratefully acknowledged.

Microscopic experimental study on the effects of NaCl concentration on the self-preservation effect of methane hydrates under 268.15 K

Yu-Jie Zhu¹, Yu-Zhou Chen¹, Yan Xie², Jin-Rong Zhong³, Xiao-Hui Wang¹, Peng Xiao¹, Yi-Fei Sun¹, Chang-Yu Sun¹, Guang-Jin Chen¹

1. State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing 102249, China;
2. Research Centre of Ecology &Environment for Coastal Area and Deep Sea, Guangdong University of Technology, Guangzhou 510006, China;
3. School of Chemistry and Food Engineering, Changsha University of Science and Technology, Changsha 410114, China

Received:2023-12-22 Revised:2024-04-10 Accepted:2024-04-15 Online:2024-11-21 Published:2024-05-28
Contact: Xiao-Hui Wang,E-mail:xh.wang@cup.edu.cn;Chang-Yu Sun,E-mail:cysun@cup.edu.cn
Supported by:
The financial support received from the Basic Research Program of Qinghai Province (2023-ZJ-703), the National Natural Science Foundation of China (22178379, 42206223), and the National Key Research and Development Program of China (2021YFC2800902) is gratefully acknowledged.

摘要/Abstract

摘要： It is known that salt ions are abundant in the natural environment where natural gas hydrates are located; thus, it is essential to investigate the self-preservation effect of salt ions on methane hydrates. The dissociation behaviors of gas hydrates formed from various NaCl concentration solutions in a quartz sand system at 268.15 K were investigated to reveal the microscopic mechanism of the self-preservation effect under different salt concentrations. Results showed that as the salt concentration rises, the initial rate of hydrate decomposition quickens. Methane hydrate hardly shows self-preservation ability in the 3.35% (mass) NaCl and seawater systems at 268.15 K. Combined the morphology of hydrate observed by the confocal microscope with results obtained from in situ Raman spectroscopy, it was found that during the initial decomposition stage of gas hydrate below the ice point, gas hydrate firstly converts into liquid water and gas molecules, then turns from water to solid ice rather than directly transforming into solid ice and gas molecules. The presence of salt ions interferes with the ability of liquid water to condense into solid ice. The results of this study provide an important guide for the mechanism and application of the self-preservation effect on the storage and transport of gas and the exploitation of natural gas hydrates.

关键词: Gas hydrate, Self-preservation, Salinity, In situ Raman spectroscopy, Endothermic behavior, Dissociation

Abstract: It is known that salt ions are abundant in the natural environment where natural gas hydrates are located; thus, it is essential to investigate the self-preservation effect of salt ions on methane hydrates. The dissociation behaviors of gas hydrates formed from various NaCl concentration solutions in a quartz sand system at 268.15 K were investigated to reveal the microscopic mechanism of the self-preservation effect under different salt concentrations. Results showed that as the salt concentration rises, the initial rate of hydrate decomposition quickens. Methane hydrate hardly shows self-preservation ability in the 3.35% (mass) NaCl and seawater systems at 268.15 K. Combined the morphology of hydrate observed by the confocal microscope with results obtained from in situ Raman spectroscopy, it was found that during the initial decomposition stage of gas hydrate below the ice point, gas hydrate firstly converts into liquid water and gas molecules, then turns from water to solid ice rather than directly transforming into solid ice and gas molecules. The presence of salt ions interferes with the ability of liquid water to condense into solid ice. The results of this study provide an important guide for the mechanism and application of the self-preservation effect on the storage and transport of gas and the exploitation of natural gas hydrates.

Key words: Gas hydrate, Self-preservation, Salinity, In situ Raman spectroscopy, Endothermic behavior, Dissociation

Yu-Jie Zhu, Yu-Zhou Chen, Yan Xie, Jin-Rong Zhong, Xiao-Hui Wang, Peng Xiao, Yi-Fei Sun, Chang-Yu Sun, Guang-Jin Chen. Microscopic experimental study on the effects of NaCl concentration on the self-preservation effect of methane hydrates under 268.15 K[J]. 中国化学工程学报, 2024, 73(9): 1-14.

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Microscopic experimental study on the effects of NaCl concentration on the self-preservation effect of methane hydrates under 268.15 K

Microscopic experimental study on the effects of NaCl concentration on the self-preservation effect of methane hydrates under 268.15 K

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