Structure and Composition of CO2/H2 and CO2/H2/C3H8 Hydrate in Relation to Simultaneous CO2 Capture and H2 Production

被引:140
作者
Kumar, Rajnish [1 ,2 ]
Englezos, Peter [1 ]
Moudrakovski, Igor [2 ]
Ripmeester, John A. [2 ]
机构
[1] Univ British Columbia, Dept Chem & Biol Engn, Vancouver, BC V6T 1Z3, Canada
[2] Natl Res Council Canada, Steacie Inst Mol Sci, Ottawa, ON K1A 0R6, Canada
基金
加拿大自然科学与工程研究理事会;
关键词
CLATHRATE HYDRATE; HYDROGEN STORAGE; CARBON-DIOXIDE; PHASE-EQUILIBRIA; SPECTROSCOPY; MIXTURES; KINETICS; DIFFRACTION; CLUSTERS;
D O I
10.1002/aic.11844
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
Gas hydrates from a (40/60 mol %) CO2/H-2 mixture, and from a (38.2/59.2/2.6 mol %) CO2/H-2/C3H8 mixture, were synthesized using ice powder. The gas uptake curves were determined from pressure drop measurements and samples were analyzed using spectroscopic techniques to identify the structure and determine the cage occupancies. Powder X-ray diffraction (PXRD) analysis at -110 degrees C was used to determine the crystal structure. From the PXRD measurement it was found that the CO2/H-2 hydrate is structure I and shows a self-preservation behavior similar to that of CO2 hydrate. The ternary gas mixture was found to form pure structure II hydrate at 3.8 MPa. We have applied attenuated total reflection infrared spectroscopic analysis to measure the CO2 distribution over the large and small cavities. H-1 MAS NMR and Raman were used to follow H-2 enclathration in the small cages of structure I, as well as structure II hydrate. (C) 2009 American Institute of Chemical Engineers AIChE J, 55: 1584-1594, 2009
引用
收藏
页码:1584 / 1594
页数:11
相关论文
共 46 条
[1]   NMR shielding constants for hydrogen guest molecules in structure II clathrates [J].
Alavi, S ;
Ripmeester, JA ;
Klug, DD .
JOURNAL OF CHEMICAL PHYSICS, 2005, 123 (05)
[2]   Molecular-dynamics study of structure II hydrogen clathrates [J].
Alavi, S ;
Ripmeester, JA ;
Klug, DD .
JOURNAL OF CHEMICAL PHYSICS, 2005, 123 (02)
[3]   Hydrogen-gas migration through clathrate hydrate cages [J].
Alavi, Saman ;
Ripmeester, John A. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2007, 46 (32) :6102-6105
[4]   Phase relations and binary clathrate hydrate formation in the system H2-THF-H2O [J].
Anderson, Ross ;
Chapoy, Antonin ;
Tohidi, Bahman .
LANGMUIR, 2007, 23 (06) :3440-3444
[5]  
Davidson D., 1973, Water in Crystalline Hydrates Aqueous Solutions of Simple Nonelectrolytes, P115
[6]   CARBON-DIOXIDE CLATHRATE HYDRATE EPITAXIAL-GROWTH - SPECTROSCOPIC EVIDENCE FOR FORMATION OF THE SIMPLE TYPE-II CO2 HYDRATE [J].
FLEYFEL, F ;
DEVLIN, JP .
JOURNAL OF PHYSICAL CHEMISTRY, 1991, 95 (09) :3811-3815
[7]   Stable low-pressure hydrogen clusters stored in a binary clathrate hydrate [J].
Florusse, LJ ;
Peters, CJ ;
Schoonman, J ;
Hester, KC ;
Koh, CA ;
Dec, SF ;
Marsh, KN ;
Sloan, ED .
SCIENCE, 2004, 306 (5695) :469-471
[8]   Phase equilibria for H2 plus CO2 plus tetrahydrofuran plus water mixtures containing gas hydrates [J].
Hashimoto, Shunsuke ;
Murayama, Shu ;
Sugahara, Takeshi ;
Ohgaki, Kazunari .
JOURNAL OF CHEMICAL AND ENGINEERING DATA, 2006, 51 (05) :1884-1886
[9]   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
[10]   Molecular hydrogen occupancy in binary THF-H2 clathrate hydrates by high resolution neutron diffraction [J].
Hester, Keith C. ;
Strobel, Timothy A. ;
Sloan, E. Dendy ;
Koh, Carolyn A. ;
Huq, Ashfia ;
Schultz, Arthur J. .
JOURNAL OF PHYSICAL CHEMISTRY B, 2006, 110 (29) :14024-14027