烃类水合物导热特性的分子动力学模拟

doi:10.3969/j.issn.0438-1157.2014.03.004

化工学报 ›› 2014, Vol. 65 ›› Issue (3): 792-796.DOI: 10.3969/j.issn.0438-1157.2014.03.004

烃类水合物导热特性的分子动力学模拟

万丽华^1,2, 梁德青^1,2, 关进安^1,2

1 中国科学院广州能源研究所, 广东广州 510640;
2 中国科学院可再生能源与天然气水合物重点实验室, 广东广州 510640

收稿日期:2013-06-26 修回日期:2013-12-14 出版日期:2014-03-05 发布日期:2014-03-05
通讯作者: 梁德青
作者简介:万丽华（1976—），女，博士，副研究员。
基金资助:
国家自然科学基金项目（51106163， 51206169）；中国科学院知识创新工程（KGZD-EW-301）；国家自然科学基金-广东省联合基金项目（U0933004）。

Characteristic of thermal conduction in hydrocarbon hydrates using molecular dynamics method

WAN Lihua^1,2, LIANG Deqing^1,2, GUAN Jin'an^1,2

1 Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, Guangdong, China;
2 Key Laboratory of Renewable Energy and Gas Hydrate, Chinese Academy of Sciences, Guangzhou 510640, Guangdong, China

Received:2013-06-26 Revised:2013-12-14 Online:2014-03-05 Published:2014-03-05
Supported by:
supported by the National Natural Science Foundation of China (51106163, 51206169), the Knowledge Innovation Program in Chinese Academy of Science (KGZD-EW-301) and the National Natural Science Foundation of China-Guangdong (U0933004).

摘要/Abstract

摘要： 采用分子动力学模拟方法Green-Kubo理论计算了263.15 K、3 MPa，sⅠ乙烷水合物、乙烯水合物的导热，给出密度和热导率值。从主客体分子和晶体结构（致密性、规整程度）对导热的影响等角度研究了烃类水合物（甲烷水合物、乙烷水合物、乙烯水合物）导热的特性。结果显示化学性质相似、分子量相差不大的烃类形成的水合物，其导热具有相似的温度压力依赖关系和晶体结构相关关系。对于sⅠ型水合物，水分子对水合物导热的影响远远超过客体分子对导热的影响。水合物的分子量越大，水合物密度越大，热导率越大。水合物晶体越致密、晶格越规整，热导率越大。

关键词: 水合物, 热传导, 分子模拟, Green-Kubo理论, 晶体结构, 分子量, 规整程度

Abstract: Equilibrium molecular dynamics simulations and the Green-Kubo method are used to the sⅠ hydrates of methane, ethane and ethene to study their thermal conduction at temperature 263.15 K and pressure 3 MPa. Thermal conductivities and mean densities of the hydrates are obtained. Characteristics of thermal conduction in hydrates of hydrocarbon such as methane, ethane or ethene are studied for the effects of host and guest molecules and compactness and regularity of the crystal lattice on thermal conduction. The results show that thermal conduction is similar for the hydrocarbon hydrates that resembles chemically with indistinct difference in molecular weight. The thermal conduction of these hydrocarbon hydrates has similar temperature and pressure dependence and similar crystal structure correlation. The influence of water on thermal conductivity of sⅠ gas hydrates goes far beyond the effect of guest molecules on it. With higher mean molecular weight in hydrates, higher densities are more conducive to enhance the thermal conductivity. More compact crystal lattices improve thermal conductivities. With more regular lattice structures, phonon mean free paths are longer, so that the thermal conductivity of hydrate increases.

Key words: hydrate, heat conduction, molecular simulation, Green-Kubo method, lattice structures, molecular weight, regularity of crystal lattice

中图分类号:

O482.2⁺2

万丽华, 梁德青, 关进安. 烃类水合物导热特性的分子动力学模拟[J]. 化工学报, 2014, 65(3): 792-796.

WAN Lihua, LIANG Deqing, GUAN Jin'an. Characteristic of thermal conduction in hydrocarbon hydrates using molecular dynamics method[J]. CIESC Journal, 2014, 65(3): 792-796.

参考文献 23

[1]	Cook J G, Laubitz M J. The thermal conductivity of two clathrate hydrates//Proceedings of 17th International Thermal Conductivity Conference[C]. Gaithersburg, 1981: 13-40
[2]	Waite W F, Pinkston J, Kirby S H. Preliminary laboratory thermal conductivity measurements in pure methane hydrate and methane hydrate-sediment mixtures//Proceedings of the Fourth International Conference on Gas Hydrate[C]. Yokohama, 2002
[3]	Huang D Z, Fan S S. Thermal conductivity of methane hydrate formed from sodium dodecyl sulfate solution[J]. J. Chem. Eng. Data, 2004, 49: 1479-1482
[4]	Stoll R D, Bryan G M. Physical properties of sediments containing gas hydrates[J]. J. Geo. Phys. Res., 1979, 84: 1629-1634
[5]	Yue Yingjie(岳英洁), Ye Yuguang(业渝光), Diao Shaobo(刁少波), Zhao Guangtao(赵广涛). Preliminary experiment on thermal properties of the sediments containing gas hydrate[J]. Mar. Geol. Lett.(海洋地质动态), 2007, 23(5):35-37
[6]	Shi Lei(石磊). Study on gas hydrate conductivity[D]. Beijing: Graduate School of Chinese Academy of Sciences, 2002
[7]	Cook J G, Leaist D G. An exploratory study of the thermal conductivity of methane hydrate[J]. Geo. Phys. Res. Lett., 1983, 10: 397-399
[8]	Wan Lihua(万丽华), Liang Deqing(梁德青), Wu Nengyou(吴能友), Guan Jin'an(关进安). Molecular dynamics simulation on influence of guest molecule number on methane hydrate thermal performance[J]. CIESC Journal (化工学报), 2012,63(2):382-386
[9]	Wan L H, Liang D Q, Wu N Y, Guan J A. Molecular dynamics simulations of the mechanisms of thermal conduction in methane hydrates[J].Sci. China Chem., 2012,55(1): 167-174
[10]	Jiang H, Myshakin E M, Jordan K D, Warzinski R P. Molecular dynamics simulations of the thermal conductivity of methane hydrate[J]. J. Phys. Chem. B, 2008, 112: 10207-10216
[11]	Rosenbaum E J, English N J, Johnson J K, Shaw D W, Warzinski R P. Thermal conductivity of methane hydrate from experiment and molecular simulation[J]. J. Phys. Chem. B, 2007, 111: 13194-13250
[12]	English N J. Effects of electrostatics techniques on the estimation of thermal conductivity via equilibrium molecular dynamics simulation: application to methane hydrates[J]. Mol. Phys., 2008, 106(15): 1887-1898
[13]	Ross R G, Andersson P. Clathrate and other solid phases in the tetrahydrofuran-water system: thermal conductivity and heat capacity under pressure[J].Can. J. Chem., 1982, 60: 881-892
[14]	Tse J S, White M A. Origin of glassy crystalline behavior in the thermal properties of clathrate hydrates: a thermal conductivity study of tetrahydrofuran hydrate[J]. J.Phys.Chem., 1988, 92: 5006-5011
[15]	Vogelsang R, Hoheisel C. Thermal conductivity of a binary-liquid mixture studies by molecular dynamics with the use of Lennard-Jones potentials[J]. Phys.Rev. A, 1987, 35: 3487-3491
[16]	Kirchner M T, Boese R, Billups W E, Norman L R. Gas hydrate single-crystal structure analysis[J]. J. Am. Chem. Soc.,2004,126: 9407-9412
[17]	Chelling P K, Phillpot S R, Keblinski P. Comparison of atomic-level simulation methods for computing thermal conductivity[J]. Phys. Rev. B, 2002, 65(14): 144306/1-144306/12
[18]	Mahoney M W, Jorgensen W L. A five-site model for liquid water and the reproduction of the density anomaly by rigid nonpolarizable potential functions[J]. J. Chem. Phys., 2000, 112: 8910-8922
[19]	Jorgensen W L, Madura J D, Swenson C J. Optimized intermolecular potential functions for liquid hydrocarbons[J]. J. Am. Chem. Soc., 1984, 106: 6638-6646
[20]	Fan Shuanshi(樊栓狮). Natural Gas Storage and Transportation in Hydrate Form(天然气水合物储存与运输技术)[M]. Beijing: Chemical Industry Press, 2005
[21]	C.Ш.БЬIK. ГAOBЬIE ГИДPAT(气体水合物)[M]. Wang Mengshun(王梦舜), trans. Beijing: Petroleum Industry Press, 1987
[22]	Sloan E D. Clathrate Hydrates of Natural Gases[M]. 2nd ed. New York: Marcel Dekker, Inc., 1998
[23]	Chialvo A A, Houssa M, Cummings P T. Molecular dynamics study of the structure and thermophysical properties of model sI clathrate hydrates[J]. J. Phys. Chem. B,2002, 106: 442-451

烃类水合物导热特性的分子动力学模拟

Characteristic of thermal conduction in hydrocarbon hydrates using molecular dynamics method

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