Anomalous Energetics in Tetrahydrofuran Clathrate Hydrate Revealed by X-ray Compton Scattering

被引：15

作者：

Lehmkuehler, Felix ^{[1
]}

Sakko, Arto ^{[2
]}

Sternemann, Christian ^{[1
]}

Hakala, Mikko ^{[2
]}

Nygard, Kim ^{[3
]}

Sahle, Christoph J. ^{[1
]}

Galambosi, Szabolcs ^{[2
]}

Steinke, Ingo ^{[1
]}

Tiemeyer, Sebastian ^{[1
]}

Nyrow, Alexander ^{[1
]}

Buslaps, Thomas ^{[4
]}

Pontoni, Diego ^{[4
]}

Tolan, Metin ^{[1
]}

Hamalainen, Keijo ^{[2
]}

机构：

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

[2] Univ Helsinki, Dept Phys, FIN-00014 Helsinki, Finland

[3] Paul Scherrer Inst, CH-5232 Villigen, Switzerland

[4] European Synchrotron Radiat Facil, F-38043 Grenoble 9, France

来源：

JOURNAL OF PHYSICAL CHEMISTRY LETTERS | 2010年 / 1卷 / 19期

基金：

芬兰科学院;

关键词：

THERMAL EXPANSIVITY; ETHYLENE-OXIDE;

D O I：

10.1021/jz1010362

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：

Changes in the ground-state electron momentum density of tetra-hydrofuran clathrate hydrate are studied in a temperature range between 93 and 275 K by means of X-ray Compton scattering. At temperatures above 253 K, large rather unexpected differences from the Compton profiles of ice are observed. Configurational enthalpies are extracted and exhibit a rapid rise above 253 K, whereas a constant configurational heat capacity of 0.23 +/- 0.07 J g(-1) K(-1) is found below 253 K. Density functional theory calculations suggest that this abomalous behavior originates from the structural change of the hydrate, however, no indication was found for the formation of hydrogen bonds between tetrahydro-furan and water molecules.

引用

页码：2832 / 2836

页数：5

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