The Carbon Dioxide-Water Interface at Conditions of Gas Hydrate Formation

被引：63

作者：

Lehmkuehler, Felix ^{[1
]}

Paulus, Michael ^{[1
]}

Sternemann, Christian ^{[1
]}

Lietz, Daniela ^{[1
]}

Venturini, Federica ^{[2
]}

Gutt, Christian ^{[3
]}

Tolan, Metin ^{[1
]}

机构：

[1] Tech Univ Dortmund, Fak Phys, DELTA, D-44221 Dortmund, Germany

[2] ESRF, F-38043 Grenoble, France

[3] DESY, HAYSLAB, D-22607 Hamburg, Germany

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2009年 / 131卷 / 02期

关键词：

X-RAY REFLECTIVITY; MOLECULAR-DYNAMICS; NUCLEATION MECHANISMS; CLATHRATE-HYDRATE; LIQUID WATER; CO2; CLUSTERS;

D O I：

10.1021/ja806211r

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The structure of the carbon dioxide-water interface was analyzed by X-ray diffraction and reflectivity at temperature and pressure conditions which allow the formation of gas hydrate. The water-gaseous CO(2) and the water-liquid CO(2) interface were examined. The two interfaces show a very different behavior with respect to the formation of gas hydrate. While the liquid-gas interface exhibits the formation of thin liquid CO(2) layers on the water surface, the formation of small clusters of gas hydrate was observed at the liquid-liquid interface. The data obtained from both interfaces points to a gas hydrate formation process which may be explained by the so-called local structuring hypothesis.

引用

页码：585 / 589

页数：5

共 31 条

[1]

[Anonymous], 1999, XRAY SCATTERING SOFT

[2]

[Anonymous], 2001, ELEMENTS MODERN XRAY

[3] CAPILLARY WAVES ON THE SURFACE OF SIMPLE LIQUIDS MEASURED BY X-RAY REFLECTIVITY [J].

BRASLAU, A ;

PERSHAN, PS ;

SWISLOW, G ;

OCKO, BM ;

ALSNIELSEN, J .

PHYSICAL REVIEW A, 1988, 38 (05) :2457-2470

[4] Direct experiments on the ocean disposal of fossil fuel CO2 [J].

Brewer, PG ;

Friederich, C ;

Peltzer, ET ;

Orr, FM .

SCIENCE, 1999, 284 (5416) :943-945

[5] 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

[6] Lifetimes of cagelike water clusters immersed in bulk liquid water: A molecular dynamics study on gas hydrate nucleation mechanisms [J].

Guo, GJ ;

Zhang, YG ;

Zhao, YJ ;

Refson, K ;

Shan, GH .

JOURNAL OF CHEMICAL PHYSICS, 2004, 121 (03) :1542-1547

[7] Effect of methane adsorption on the lifetime of a dodecahedral water cluster immersed in liquid water: A molecular dynamics study on the hydrate nucleation mechanisms [J].

Guo, Guang-Jun ;

Zhang, Yi-Gang ;

Liu, Hua .

JOURNAL OF PHYSICAL CHEMISTRY C, 2007, 111 (06) :2595-2606

[8] CO2 clathrate-hydrate formation and its mechanism by molecular dynamics simulation [J].

Hirai, S ;

Okazaki, K ;

Tabe, Y ;

Kawamura, K .

ENERGY CONVERSION AND MANAGEMENT, 1997, 38 :S301-S306

[9] X-ray optics for liquid surface/interface spectrometers [J].

Honkimaeki, V. ;

Reichert, H. ;

Okasinski, J. S. ;

Dosch, H. .

JOURNAL OF SYNCHROTRON RADIATION, 2006, 13 :426-431

[10] Recovery of CO2 from flue gas using gas hydrate:: Thermodynamic verification through phase equilibrium measurements [J].

Kang, SP ;

Lee, H .

ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2000, 34 (20) :4397-4400

← 1 2 3 4 →