光谱学与光谱分析, 2015, 35 (11): 2996, 网络出版: 2016-02-02   

激光拉曼光谱在气体水合物研究中的应用

Laser Raman Spectroscopy and Its Application in Gas Hydrate Studies
作者单位
1 中国科学院广州地球化学研究所, 广东 广州 510640
2 中国科学院广州能源研究所, 广东 广州 510640
3 中国科学院大学, 北京 100049
4 青岛海洋地质研究所, 山东 青岛 266071
5 北京大学工学院, 北京 100871
摘要
天然气水合物是一种重要的潜在能源。 用激光拉曼光谱法表征气体水合物能够为研究水合物形成机理和开采方法提供重要信息。 系统介绍了激光拉曼光谱法的基本原理, 综述了激光拉曼光谱仪在气体水合物微观表征上的各种实际应用。 通过激光拉曼测试可分析水合物气体组成、 推测结构类型, 再利用经验公式或者相对定量法可计算出其大/小笼的气体占有率和水合数;利用原位拉曼技术可以观测水合物形成和分解的微观过程, 解析气体分子进入和离开笼子的进程、 进行水合物形成和分解过程中气体浓度变化及水合物形成过程中气体溶解度的测定, 辨识水合物系统中的相变过程, 进而研究水合物形成和分解动力学;激光拉曼光谱法还可用于研究超高压条件下气体水合物的结构及其变化过程。 原位拉曼光谱能够对深海天然气水合物及其环境在原位进行表征;利用拉曼成像技术可以对水合物晶体表面进行系统测定, 探求气体组分在晶体表面的分布。 随着激光拉曼技术的发展及与其他设备联用水平的提高, 激光拉曼光谱仪向便携, 高灵敏度发展, 能够更广泛深入地进行气体水合物微观研究。
Abstract
Gas hydrates are important potential energy resources. Microstructural characterization of gas hydrate can provide information to study the mechanism of gas hydrate formation and to support the exploitation and application of gas hydrate technology. This article systemly introduces the basic principle of laser Raman spectroscopy and summarizes its application in gas hydrate studies. Based on Raman results, not only can the information about gas composition and structural type be deduced, but also the occupancies of large and small cages and even hydration number can be calculated from the relative intensities of Raman peaks. By using the in-situ analytical technology, laser Raman specstropy can be applied to characterize the formation and decomposition processes of gas hydrate at microscale, for example the enclathration and leaving of gas molecules into/from its cages, to monitor the changes in gas concentration and gas solubility during hydrate formation and decomposition, and to identify phase changes in the study system. Laser Raman in-situ analytical technology has also been used in determination of hydrate structure and understanding its changing process under the conditions of ultra high pressure. Deep-sea in-situ Raman spectrometer can be employed for the in-situ analysis of the structures of natural gas hydrate and their formation environment. Raman imaging technology can be applied to specify the characteristics of crystallization and gas distribution over hydrate surface. With the development of laser Raman technology and its combination with other instruments, it will become more powerful and play a more significant role in the microscopic study of gas hydrate.

付娟, 吴能友, 卢海龙, 邬黛黛, 苏秋成. 激光拉曼光谱在气体水合物研究中的应用[J]. 光谱学与光谱分析, 2015, 35(11): 2996. FU Juan, WU Neng-you, LU Hai-long, WU Dai-dai, SU Qiu-cheng. Laser Raman Spectroscopy and Its Application in Gas Hydrate Studies[J]. Spectroscopy and Spectral Analysis, 2015, 35(11): 2996.

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