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化学学报
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化学学报 ›› 2010, Vol. 68 ›› Issue (18): 1881-1886. 上一篇    下一篇

研究论文

南海神狐海域及祁连山冻土区天然气水合物的拉曼光谱特征

刘昌岭*,1,2，业渝光1,2，孟庆国2，卢振权3，祝有海3，刘坚4，杨胜雄4   

  1. (1国土资源部海洋油气资源与环境地质重点实验室 青岛 266071)
    (2青岛海洋地质研究所 青岛 266071)
    (3中国地质科学院矿产资源研究所 北京 100037)
    (4广州海洋地质调查局 广州 510760)
  • 投稿日期:2010-02-05 修回日期:2010-05-10 发布日期:2010-05-25
  • 通讯作者: 刘昌岭 E-mail:qdliuchangling@163.com
  • 基金资助:

    国家重点基础研究发展计划;国土资源部公益性行业科研专项经费项目;我国海域天然气水合物资源调查与评价专项

Raman Spectroscopic Characteristics of Natural Gas Hydrate Recovered from Shenhu Area in South China Sea and Qilian Mountain Permafrost

Liu Changling*,1,2 Ye Yuguang1,2 Meng Qingguo2 Lu Zhenquan3 Zhu Youhai3 Liu Jian4 Yang Shengxiong4   

  1. (1 Key Laboratory of Marine Hydrocarbon Resources and Environmental Geology, Ministry of Land and Resources, Qingdao 266071)
    (2 Qingdao Institute of Marine Geology, Qingdao 266071)
    (3 Institute of Mineral Resources, Chinese Academy of Geological Sciences, Beijing 100037)
    (4 Guangzhou Marine Geological Survey, Guangzhou 510760)
  • Received:2010-02-05 Revised:2010-05-10 Published:2010-05-25
  • Contact: Liu changling E-mail:qdliuchangling@163.com

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采用显微激光拉曼光谱对我国在南海神狐海域及祁连山冻土区首次钻获的天然气水合物实物样品进行了详细的研究, 探讨了其笼型结构特征及其气体组成. 结果表明, 南海神狐海域天然气水合物样品是典型的I型结构(sI)水合物, 气体组分主要是甲烷, 占99%以上; 水合物大笼的甲烷占有率大于99%, 小笼为86%, 水合指数为5.99. 祁连山冻土区天然气水合物气体组分相对复杂, 主要成分除甲烷外(70%左右), 还有相当数量的乙烷、丙烷及丁烷等烃类气体, 从拉曼谱图上可初步判断其为II型结构(sII)水合物; 水合物的小、大笼的甲烷占有率的比值(θS/θL)为26.38, 远远大于南海神弧海域水合物的0.87, 这主要是由于祁连山水合物气体组分中的大分子(乙烷、丙烷及丁烷等)优先占据水合物的大笼, 大大减少了大笼中甲烷分子的数量.

关键词: 天然气水合物, 显微激光拉曼光谱, 神狐海域, 祁连山冻土区

Natural gas hydrate samples were firstly recovered from Shenhu Area of South China Sea (SH-GH) and Qilian mountain permafrost (QLM-GH) in China. In this paper, laser micro-Raman spectroscopy was used to investigate the two kinds of samples to reveal the structural characteristics and the gas composition of these natural gas hydrates. The results show that SH-GH is typically structure I (sI) hydrate. Methane gas is a dominant component which accounts for more than 99% of all the guest gas. The cage occupancy of methane is larger than 99% for large cages while 86% for small cages, with the hydration number of approximately 5.99 by Raman method. In comparison, QLM-GH is formed by relatively complicated gas components. Except for methane (about 70%), there are also considerable amounts of ethane, propane and butane. It is presumed preliminarily that GH-QLM is structure II (sII) hydrate based on its Raman spectrum, with the cage occupancy ratio of methane for small to large cage (θS/θL) of 26.38, which is much larger than that of GH-SH (0.87). This is mainly because the lager molecules (i.e. ethane, propane and butane) in QLM-GH preferentially occupy the large cages and thus greatly diminish methane molecules in large cages.

Key words: gas hydrate, laser micro-Raman spectrometry, Shenhu Area, qilian Mountain permafrost