Structure and dynamics of hydrogen molecules in the novel clathrate hydrate by high pressure neutron diffraction

被引：255
|
作者：
Lokshin, KA
Zhao, YS
He, DW
Mao, WL
Mao, HK
Hemley, RJ
Lobanov, MV
Greenblatt, M
机构：
[1] Los Alamos Natl Lab, LANSCE 12, Los Alamos, NM 87544 USA
[2] Carnegie Inst Sci, Geophys Lab, Washington, DC 20015 USA
[3] Univ Chicago, Dept Geophys Sci, Chicago, IL 60637 USA
[4] Rutgers State Univ, Dept Chem & Biol Chem, Piscataway, NJ 08854 USA
来源：
PHYSICAL REVIEW LETTERS | 2004年 / 93卷 / 12期
基金：
美国国家科学基金会;
关键词：
D O I：
10.1103/PhysRevLett.93.125503
中图分类号：
O4 [物理学];
学科分类号：
0702 ;
摘要：
The D-2 clathrate hydrate crystal structure was determined as a function of temperature and pressure by neutron diffraction for the first time. The hydrogen occupancy in the (32+X)H-2.136H(2)O, x=0-16 clathrate can be reversibly varied by changing the large (hexakaidecahedral) cage occupancy between two and four molecules, while remaining single occupancy of the small (dodecahedral) cage. Above 130-160 K, the guest D-2 molecules were found in the delocalized state, rotating around the centers of the cages. Decrease of temperature results in rotation freezing followed by a complete localization below 50 K.
引用
收藏
页码：125503 / 1
页数：4
相关论文
共 50 条
  • [41] Disorder of Hydrofluorocarbon Molecules Entrapped in the Water Cages of Structure I Clathrate Hydrate
    Takeya, Satoshi
    Udachin, Konstantin A.
    Moudrakovski, Igor L.
    Ohmura, Ryo
    Ripmeester, John A.
    [J]. CHEMISTRY-A EUROPEAN JOURNAL, 2016, 22 (22) : 7567 - 7573
  • [42] Molecular dynamics studies of structure I clathrate hydrate of carbon dioxide
    Itoh, H
    Horikawa, S
    Kawamura, K
    Uchida, T
    Hondoh, T
    Mae, S
    [J]. NGH '96 - 2ND INTERNATIONAL CONFERENCE ON NATURAL GAS HYDRATES, PROCEEDINGS, 1996, : 341 - 346
  • [43] Molecular dynamics simulation for the formation of argon clathrate-hydrate structure
    Hirai, S
    Okazaki, K
    Kuraoka, S
    Kawamura, K
    [J]. MICROSCALE THERMOPHYSICAL ENGINEERING, 1997, 1 (04): : 293 - 301
  • [44] Structure, dynamics and thermodynamic stability of high-pressure ices and clathrate hydrates
    Yagasaki, Takuma
    Himoto, Kazuhiro
    Nakamura, Tatsuya
    Matsumoto, Masakazu
    Tanaka, Hideki
    [J]. MOLECULAR SIMULATION, 2015, 41 (10-12) : 868 - 873
  • [45] Modeling the THF clathrate hydrate dynamics by combining molecular dynamics and quasi-elastic neutron scattering
    Pefoute, Eric
    Martin-Gondre, Ludovic
    Ollivier, Jacques
    Soetens, Jean-Christophe
    Russina, Margarita
    Desmedt, Arnaud
    [J]. CHEMICAL PHYSICS, 2017, 496 : 24 - 34
  • [46] Molecular hydrogen occupancy in binary THF-H2 clathrate hydrates by high resolution neutron diffraction
    Hester, Keith C.
    Strobel, Timothy A.
    Sloan, E. Dendy
    Koh, Carolyn A.
    Huq, Ashfia
    Schultz, Arthur J.
    [J]. JOURNAL OF PHYSICAL CHEMISTRY B, 2006, 110 (29): : 14024 - 14027
  • [47] Neutron diffraction study of structure I and structure II trimethylene oxide clathrate deuterate
    Rondinone, AJ
    Chakoumakos, BC
    Rawn, CJ
    Ishii, Y
    [J]. JOURNAL OF PHYSICAL CHEMISTRY B, 2003, 107 (25): : 6046 - 6050
  • [48] Revisiting the magnetic structure of Holmium at high pressure by using neutron diffraction
    Pardo-Sainz, M.
    Cova, F.
    Rodriguez-Velamazan, J. A.
    Puente-Orench, I.
    Kousaka, Y.
    Mito, M.
    Campo, J.
    [J]. SCIENTIFIC REPORTS, 2023, 13 (01)
  • [49] Molecular-Dynamics and First-Principles Calculations of Raman Spectra and Molecular and Electronic Structure of Hydrogen Clusters in Hydrogen Clathrate Hydrate
    Wang, Jianwei
    Lu, Hailong
    Ripmeester, John A.
    Becker, Udo
    [J]. JOURNAL OF PHYSICAL CHEMISTRY C, 2010, 114 (49): : 21042 - 21050
  • [50] Revisiting the magnetic structure of Holmium at high pressure by using neutron diffraction
    M. Pardo-Sainz
    F. Cova
    J. A. Rodríguez-Velamazán
    I. Puente-Orench
    Y. Kousaka
    M. Mito
    J. Campo
    [J]. Scientific Reports, 13
12345