SDS对甲烷水合物生成动力学和微观结构的影响

doi:10.11949/j.issn.0438-1157.20170687

化工学报 ›› 2017, Vol. 68 ›› Issue (12): 4802-4808.DOI: 10.11949/j.issn.0438-1157.20170687

SDS对甲烷水合物生成动力学和微观结构的影响

丁家祥^1,2,3,4,5, 史伶俐^1,2,3,4, 申小冬^1,2,3,4,5, 梁德青^1,2,3,4

1 中国科学院天然气水合物重点实验室, 广东广州 510640;
2 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;
3 中国科学院广州能源研究所, 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;
5 中国科学院大学, 北京 100049

收稿日期:2017-05-26 修回日期:2017-07-24 出版日期:2017-12-05 发布日期:2017-12-05
通讯作者: 梁德青
基金资助:
国家自然科学基金项目（51376182）。

SDS effect on formation kinetics and microstructure of methane hydrate

DING Jiaxiang^1,2,3,4,5, SHI Lingli^1,2,3,4, SHEN Xiaodong^1,2,3,4,5, LIANG Deqing^1,2,3,4

1 CAS Key Laboratory of Gas Hydrate, Guangzhou 510640, Guangdong, China;
2 Guangdong Provincial Key Laboratory of New and Renewable Energy Research and Development, Guangzhou 510640, Guangdong, China;
3 Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, Guangdong, China;
4 Guangzhou Center for Gas Hydrate Research, Chinese Academy of Sciences, Guangzhou 510640, Guangdong, China;
5 University of Chinese Academy of Sciences, Beijing 100049, China

Received:2017-05-26 Revised:2017-07-24 Online:2017-12-05 Published:2017-12-05
Supported by:
supported by the National Natural Science Foundation of China (51376182).

摘要/Abstract

摘要：

表面活性剂是促进水合物生成的有效手段之一。在高压反应釜中研究了十二烷基硫酸钠（SDS）对水合物生成过程的动力学影响，利用XRD和拉曼光谱探究了SDS存在条件下水合物的微观结构。宏观结果表明SDS缩短了诱导时间，加快了水合物生长速率。微观结果表明SDS没有影响sI型水合物的晶型结构，晶面间距与理想sI型水合物及纯水甲烷对比误差在千分之几。水合物中甲烷在大笼小笼中的拉曼位移分别为2904和2915 cm^-1，SDS没有改变大笼小笼结构。大笼绝对占有率（q_L）接近饱和时，SDS可以进一步提高小笼绝对占有率（q_S），从微观角度证明了SDS可以减少水合数，提高储气率。

关键词: 水合物, 表面活性剂, 储气率, 动力学, 绝对占有率

Abstract:

Surfactants is one of the effective methods to promote hydrate formation. The influence of Sodium dodecyl sulfate (SDS) on the formation of hydrate was studied in an autoclave. The microscopic properties for SDS hydrate samples were detected with Raman spectroscopy and powder X-ray diffraction. It was found that the presence of SDS decreased the induction time and enhanced the hydrate growth rate. The microcosmic results showed that the presence of SDS did not change the sI-type hydrate lattice structure and had less impact (a few thousandths) on the crystal spacing compared with ideal sI-type structure and pure methane hydrate. The Raman shift of C-H stretching mode from CH₄ encapsulated in large and small cages are all 2904 and 2915 cm^-1, which illustrate SDS did not change the large and small cages structure. SDS improved the absolute small cages occupancy (q_L) as the absolute large cages occupancy (q_S) approached saturation, and this is also demonstrated that SDS can reduce hydration number and increase storage capacity.

Key words: hydrate, surfactants, storage capacity, kinetics, absolute occupancy

中图分类号:

TE89

丁家祥, 史伶俐, 申小冬, 梁德青. SDS对甲烷水合物生成动力学和微观结构的影响[J]. 化工学报, 2017, 68(12): 4802-4808.

DING Jiaxiang, SHI Lingli, SHEN Xiaodong, LIANG Deqing. SDS effect on formation kinetics and microstructure of methane hydrate[J]. CIESC Journal, 2017, 68(12): 4802-4808.

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SDS对甲烷水合物生成动力学和微观结构的影响

SDS effect on formation kinetics and microstructure of methane hydrate

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