NMR study of methane plus ethane structure I hydrate decomposition

被引:28
作者
Dec, Steven F. [1 ]
Bowler, Kristen E. [1 ]
Stadterman, Laura L. [1 ]
Koh, Carolyn A. [1 ]
Sloan, E. Dendy, Jr. [1 ]
机构
[1] Colorado Sch Mines, Dept Chem Engn, Ctr Hydrate Res, Golden, CO 80401 USA
关键词
D O I
10.1021/jp070442y
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The thermally activated decomposition of methane + ethane structure I hydrate was studied with use of C-13 magic-angle spinning (MAS) NMR as a function of composition and temperature. The observed higher decomposition rate of large sI cages initially filled with ethane gas can be described in terms of a model where a distribution of sI unit cells exists such that a particular unit cell contains zero, one, or two methane molecules in the unit cell; this distribution of unit cells is combined to form the observed equilibrium composition. In this model, unit cells with zero methane molecules are the least stable and decompose more rapidly than those populated with one or two methane molecules leading to the observed overall faster decomposition rate of the large cages containing ethane molecules.
引用
收藏
页码:4297 / 4303
页数:7
相关论文
共 21 条
[1]  
DAVIDSON DW, 1986, GEOCHIM COSMOCHIM AC, V50, P619, DOI 10.1016/0016-7037(86)90110-9
[2]   Direct measure of the hydration number of aqueous methane [J].
Dec, SF ;
Bowler, KE ;
Stadterman, LL ;
Koh, CA ;
Sloan, ED .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2006, 128 (02) :414-415
[3]   EXPERIMENTAL THERMODYNAMIC PARAMETERS FOR THE PREDICTION OF NATURAL-GAS HYDRATE DISSOCIATION CONDITIONS [J].
DHARMAWARDHANA, PB ;
PARRISH, WR ;
SLOAN, ED .
INDUSTRIAL & ENGINEERING CHEMISTRY FUNDAMENTALS, 1980, 19 (04) :410-414
[4]   FOURIER TRANSFORM STUDY OF NMR SPIN-LATTICE RELAXATION BY PROGRESSIVE-SATURATION [J].
FREEMAN, R ;
HILL, HDW .
JOURNAL OF CHEMICAL PHYSICS, 1971, 54 (08) :3367-&
[5]  
FUKUSHIMA E, 1981, EXPT PULSE NMR NUTS, P169
[6]  
Genov G, 2004, AM MINERAL, V89, P1228
[7]   NMR investigation of methane hydrate dissociation [J].
Gupta, Arvind ;
Dec, Steven F. ;
Koh, Carolyn A. ;
Sloan, E. D., Jr. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2007, 111 (05) :2341-2346
[8]   Neutron diffraction studies of CO2 clathrate hydrate:: Formation from deuterated ice [J].
Henning, RW ;
Schultz, AJ ;
Thieu, V ;
Halpern, Y .
JOURNAL OF PHYSICAL CHEMISTRY A, 2000, 104 (21) :5066-5071
[9]   Methane plus propane structure II hydrate formation kinetics [J].
Kini, RA ;
Dec, SF ;
Sloan, ED .
JOURNAL OF PHYSICAL CHEMISTRY A, 2004, 108 (44) :9550-9556
[10]   Water ordering around methane during hydrate formation [J].
Koh, CA ;
Wisbey, RP ;
Wu, XP ;
Westacott, RE ;
Soper, AK .
JOURNAL OF CHEMICAL PHYSICS, 2000, 113 (15) :6390-6397