Energetics and Dynamics of H2 Adsorbed in a Nanoporous Material at Low Temperature

被引：86

作者：

Kong, Lingzhu ^{[1
]}

Roman-Perez, Guillermo ^{[2
]}

Soler, Jose M. ^{[2
]}

Langreth, David C. ^{[1
]}

机构：

[1] Rutgers State Univ, Dept Phys & Astron, Piscataway, NJ 08854 USA

[2] Univ Autonoma Madrid, Dept Fis Mat Condensada, E-28049 Madrid, Spain

来源：

PHYSICAL REVIEW LETTERS | 2009年 / 103卷 / 09期

关键词：

METAL-ORGANIC FRAMEWORKS; SECONDARY BUILDING UNITS; NEUTRON-SCATTERING; HYDROGEN; 1ST-PRINCIPLES; SITES;

D O I：

10.1103/PhysRevLett.103.096103

中图分类号：

O4 [物理学];

学科分类号：

0702 ;

摘要：

Molecular hydrogen adsorption in a nanoporous metal-organic framework structure (MOF-74) is studied via van der Waals density-functional calculations. The primary and secondary binding sites for H-2 are confirmed. The low-lying rotational and translational energy levels are calculated, based on the orientation and position dependent potential energy surface at the two binding sites. A consistent picture is obtained between the calculated rotational-translational transitions for different H-2 loadings and those measured by inelastic neutron scattering exciting the singlet to triplet (para to ortho) transition in H-2. The H-2 binding energy after zero-point energy correction due to the rotational and translational motions is predicted to be similar to 100 meV in good agreement with the experimental value of similar to 90 meV.

引用

页数：4

共 20 条

[1] Hydrogen adsorption in HKUST-1: a combined inelastic neutron scattering and first-principles study [J].

Brown, Craig M. ;

Liu, Yun ;

Yildirim, Taner ;

Peterson, Vanessa K. ;

Kepert, Cameron J. .

NANOTECHNOLOGY, 2009, 20 (20)

[2] Van der Waals density functional for general geometries -: art. no. 246401 [J].

Dion, M ;

Rydberg, H ;

Schröder, E ;

Langreth, DC ;

Lundqvist, BI .

PHYSICAL REVIEW LETTERS, 2004, 92 (24) :246401-1

[3] Modular chemistry: Secondary building units as a basis for the design of highly porous and robust metal-organic carboxylate frameworks [J].

Eddaoudi, M ;

Moler, DB ;

Li, HL ;

Chen, BL ;

Reineke, TM ;

O'Keeffe, M ;

Yaghi, OM .

ACCOUNTS OF CHEMICAL RESEARCH, 2001, 34 (04) :319-330

[4] First-principles computation of material properties: the ABINIT software project [J].

Gonze, X ;

Beuken, JM ;

Caracas, R ;

Detraux, F ;

Fuchs, M ;

Rignanese, GM ;

Sindic, L ;

Verstraete, M ;

Zerah, G ;

Jollet, F ;

Torrent, M ;

Roy, A ;

Mikami, M ;

Ghosez, P ;

Raty, JY ;

Allan, DC .

COMPUTATIONAL MATERIALS SCIENCE, 2002, 25 (03) :478-492

[5] First-principles study of the rotational transitions of H2 physisorbed over benzene [J].

Hamel, S ;

Coté, M .

JOURNAL OF CHEMICAL PHYSICS, 2004, 121 (24) :12618-12625

[6] Theoretical and experimental analysis of H2 binding in a prototypical metal-organic framework material [J].

Kong, Lingzhu ;

Cooper, Valentino R. ;

Nijem, Nour ;

Li, Kunhao ;

Li, Jing ;

Chabal, Yves J. ;

Langreth, David C. .

PHYSICAL REVIEW B, 2009, 79 (08)

[7] A density functional for sparse matter [J].

Langreth, D. C. ;

Lundqvist, B. I. ;

Chakarova-Kack, S. D. ;

Cooper, V. R. ;

Dion, M. ;

Hyldgaard, P. ;

Kelkkanen, A. ;

Kleis, J. ;

Kong, Lingzhu ;

Li, Shen ;

Moses, P. G. ;

Murray, E. ;

Puzder, A. ;

Rydberg, H. ;

Schroder, E. ;

Thonhauser, T. .

JOURNAL OF PHYSICS-CONDENSED MATTER, 2009, 21 (08)

[8] Increasing the density of adsorbed hydrogen with coordinatively unsaturated metal centers in metal-organic frameworks [J].

Liu, Yun ;

Kabbour, Houria ;

Brown, Craig M. ;

Neumann, Dan A. ;

Ahn, Channing C. .

LANGMUIR, 2008, 24 (09) :4772-4777

[9]

MURRAY ED, J CHEM THEO IN PRESS

[10] Self-consistent order-N density-functional calculations for very large systems [J].

Ordejon, P ;

Artacho, E ;

Soler, JM .

PHYSICAL REVIEW B, 1996, 53 (16) :10441-10444

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