甲烷水合物分解过程的微尺度测量

周雪冰; 刘婵娟; 罗金琼; 梁德青

doi:10.11949/j.issn.0438-1157.20180821

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甲烷水合物分解过程的微尺度测量

能源和环境工程 | 更新时间：2026-07-24

- 甲烷水合物分解过程的微尺度测量
- Microscopic measurements on methane hydrate dissociation
- 化工学报 2019年70卷第3期页码：1042-1047
- 作者机构：
  
  1.中国科学院广州能源研究所，广东广州510640
  2.中国科学院天然气水合物重点实验室，广东广州510640
  3.广东省新能源和可再生能源研究开发与应用重点实验室，广东广州510640
  4.中国科学院广州天然气水合物中心，广东广州510640
- 作者简介：
  
  周雪冰（1986—），男，博士，助理研究员，zhouxb@ms.giec.ac.cn
  梁德青（1970—），男，研究员，liangdq@ms.giec.ac.cn
- 基金信息：
  
  国家自然科学基金项目(51706230)
- DOI：10.11949/j.issn.0438-1157.20180821
  中图分类号： TK 123
- 收稿：2018-07-18，
  
  修回：2018-10-17，
  
  网络首发：2026-07-24，
  
  纸质出版：2019-03-05
- 稿件说明：
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周雪冰, 刘婵娟, 罗金琼, 梁德青. 甲烷水合物分解过程的微尺度测量[J]. 化工学报, 2019, 70(3): 1042-1047

ZHOU Xuebing, LIU Chanjuan, LUO Jinqiong, LIANG Deqing. Microscopic measurements on methane hydrate dissociation[J]. CIESC Journal, 2019, 70(3): 1042-1047
周雪冰, 刘婵娟, 罗金琼, 梁德青. 甲烷水合物分解过程的微尺度测量[J]. 化工学报, 2019, 70(3): 1042-1047 DOI： 10.11949/j.issn.0438-1157.20180821.

ZHOU Xuebing, LIU Chanjuan, LUO Jinqiong, LIANG Deqing. Microscopic measurements on methane hydrate dissociation[J]. CIESC Journal, 2019, 70(3): 1042-1047 DOI： 10.11949/j.issn.0438-1157.20180821.

摘要

实验采用激光拉曼和X射线粉末衍射(PXRD) 在253 K，常压条件下对甲烷水合物的分解过程分别进行了原位测量。研究发现，位于表层的甲烷水合物在前30～50 min内发生分解并生成Ⅰh冰相，随后表层冰相对内层水合物相的包覆引起了“自保护”效应的产生并导致甲烷水合物分解速率显著降低。分解过程中，甲烷在水合物大小笼中的含量之比始终保持在3.2左右，同时水合物晶面特征峰峰面积也按照相同的曲线下降，表明甲烷水合物以晶胞为单位进行整体分解。Ⅰh冰的各个晶面特征峰峰面积差异化的增长曲线表明形成的Ⅰh冰相倾向于片状生长，有助于在水合物表面生成一层冰膜，进而产生“自保护”效应。

Abstract

The decomposition process of methane hydrate was measured by laser Raman and X-ray powder diffraction (PXRD) at 253 K under normal pressure. The results showed that the methane hydrates at the surface dissociated into Ⅰh ice in the initial 30—50 min and then the ice film covered the hydrate phase which triggered the “self-preservation” effect and finally led to a dramatic decrease in dissociation rate of methane hydrate. During the dissociation

the ratio of methane content in large and small hydrate cages obtained from Raman spectra remained stable at around 3.2 which was generally in accord with the ratio of large to small cages in methane hydrate

while the characteristic peaks of hydrate lattice planes in the powder X-ray diffraction patterns decreased in the same profile

suggesting that the methane hydrate dissociated as a whole crystal unit. However

the characteristic peaks of Ⅰh ice lattice planes increased in different ways. The intensity of (002) plane was found to increase linearly up to 370% of its original value in 60 min while the intensity of (100) plane kept steady at about 200% of its original value after the first 20 min

indicating that the ice inclined to grow into horizontal plates instead of columnar growth. Combining with the transport characteristics of water molecules on the ice surface under low temperature

the growth of ice film covered on the inner hydrate cores was suggested to cultivate the “self-preservation” effect.

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references

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