Details
| Original language | English |
|---|---|
| Pages (from-to) | 10455-10462 |
| Number of pages | 8 |
| Journal | Journal of Physical Chemistry C |
| Volume | 121 |
| Issue number | 19 |
| Early online date | 10 May 2017 |
| Publication status | Published - 18 May 2017 |
Abstract
Adsorption and diffusion of the gas mixture H2/CH4 in the metal-organic framework (MOF) of structure type zeolitic imidazolate framework-90 (ZIF-90) are revisited. While the adsorption can successfully be examined in Gibbs ensemble Monte Carlo (GEMC) simulations using the common approximation of a rigid lattice, the dynamics of methane in ZIF-90 is remarkably influenced by the lattice flexibility. Molecular dynamics (MD) simulations not only show a strong influence of the lattice flexibility on the diffusion of methane but even find a slight structural phase transition of the lattice. This structural change appeared at higher temperatures and was not caused by the content of guest molecules like in most former discoveries of gate opening. For prediction of mixed gas ZIF-90 membrane selectivity, the adsorption and diffusion results show that the high CH4 adsorption selectivity is overcompensated by the high H2 mobility. The comparison of our results for the H2/CH4 membrane selectivity with experimental findings from mixed gas permeation through supported ZIF-90 membranes shows better agreement than other simulations that use a rigid lattice for MD. Also, the increase of the membrane selectivity by increased temperature could be found.
ASJC Scopus subject areas
- Materials Science(all)
- Electronic, Optical and Magnetic Materials
- Energy(all)
- General Energy
- Chemistry(all)
- Physical and Theoretical Chemistry
- Materials Science(all)
- Surfaces, Coatings and Films
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In: Journal of Physical Chemistry C, Vol. 121, No. 19, 18.05.2017, p. 10455-10462.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Importance of ZIF-90 Lattice Flexibility on Diffusion, Permeation, and Lattice Structure for an adsorbed H2/CH4 Gas Mixture
T2 - A Re-Examination by Gibbs Ensemble Monte Carlo and Molecular Dynamics Simulations
AU - Chokbunpiam, T.
AU - Fritzsche, S.
AU - Caro, J.
AU - Chmelik, C.
AU - Janke, W.
AU - Hannongbua, S.
N1 - Funding Information: T.C. would like to thank the Thailand Research Fund and Office of the Higher Education Commission (MRG 5980073) and Asia Research Center at Chulalongkorn University (002/ 2560). The Computational Chemistry Unit Cell (CCUC) at Department of Chemistry, Faculty of Science, Chulalongkorn University, and the computer center of the Leipzig University are acknowledged for computer resources and other facilities.
PY - 2017/5/18
Y1 - 2017/5/18
N2 - Adsorption and diffusion of the gas mixture H2/CH4 in the metal-organic framework (MOF) of structure type zeolitic imidazolate framework-90 (ZIF-90) are revisited. While the adsorption can successfully be examined in Gibbs ensemble Monte Carlo (GEMC) simulations using the common approximation of a rigid lattice, the dynamics of methane in ZIF-90 is remarkably influenced by the lattice flexibility. Molecular dynamics (MD) simulations not only show a strong influence of the lattice flexibility on the diffusion of methane but even find a slight structural phase transition of the lattice. This structural change appeared at higher temperatures and was not caused by the content of guest molecules like in most former discoveries of gate opening. For prediction of mixed gas ZIF-90 membrane selectivity, the adsorption and diffusion results show that the high CH4 adsorption selectivity is overcompensated by the high H2 mobility. The comparison of our results for the H2/CH4 membrane selectivity with experimental findings from mixed gas permeation through supported ZIF-90 membranes shows better agreement than other simulations that use a rigid lattice for MD. Also, the increase of the membrane selectivity by increased temperature could be found.
AB - Adsorption and diffusion of the gas mixture H2/CH4 in the metal-organic framework (MOF) of structure type zeolitic imidazolate framework-90 (ZIF-90) are revisited. While the adsorption can successfully be examined in Gibbs ensemble Monte Carlo (GEMC) simulations using the common approximation of a rigid lattice, the dynamics of methane in ZIF-90 is remarkably influenced by the lattice flexibility. Molecular dynamics (MD) simulations not only show a strong influence of the lattice flexibility on the diffusion of methane but even find a slight structural phase transition of the lattice. This structural change appeared at higher temperatures and was not caused by the content of guest molecules like in most former discoveries of gate opening. For prediction of mixed gas ZIF-90 membrane selectivity, the adsorption and diffusion results show that the high CH4 adsorption selectivity is overcompensated by the high H2 mobility. The comparison of our results for the H2/CH4 membrane selectivity with experimental findings from mixed gas permeation through supported ZIF-90 membranes shows better agreement than other simulations that use a rigid lattice for MD. Also, the increase of the membrane selectivity by increased temperature could be found.
UR - http://www.scopus.com/inward/record.url?scp=85020552980&partnerID=8YFLogxK
U2 - 10.1021/acs.jpcc.7b02602
DO - 10.1021/acs.jpcc.7b02602
M3 - Article
AN - SCOPUS:85020552980
VL - 121
SP - 10455
EP - 10462
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
SN - 1932-7447
IS - 19
ER -