TY - JOUR
T1 - Atomistic mechanism of the adsorption of CFCs in zeolite as investigated by Monte Carlo simulation
AU - Mizukami, Koichi
AU - Takaba, Hiromitsu
AU - Oumi, Yasunori
AU - Katagiri, Masahiko
AU - Kubo, Momoji
AU - Stirling, Andras
AU - Broclawik, Ewa
AU - Miyamoto, Akira
AU - Kobayashi, Satoru
AU - Kushiyama, Satoshi
AU - Mizuno, Koichi
PY - 1997
Y1 - 1997
N2 - We studied the adsorption mechanism of CF2Cl2 in CsNaY zeolite by using grand canonical Monte Carlo (GCMC) method. The accurate distribution of Al3+, Cs+, and Na+ in the CsNaY (Si/Al = 2.43) was obtained from molecular dynamics (MD) calculations and NMR simulation, while the potential parameters of the CF2Cl2 were determined by density functional theory (DFT) calculations. The experimental adsorption isotherm of the CF2Cl2 in the CsNaY was fully reproduced by the GCMC simulations. Furthermore, computer graphics (CG) visualization of the calculated results revealed the presence of two different mechanisms of CF2Cl2 adsorption in the CsNaY : (1) at low pressure, the CF2Cl2 selectively and drastically adsorbed at the Cs+ cations of the CsNaY : (2) at high pressure, the aggregation of the CF2Cl2 in the super cages of the CsNaY occurred. These results indicate that our new methodology, i. e. the combination of GCMC, MD, NMR simulation, DFT, and CG, is effective and useful not only to reproduce the experimental adsorption isotherm of chlorofluorocarbons in zeolites but also to clarify the atomistic mechanism of the adsorption, which cannot be obtained experimentally.
AB - We studied the adsorption mechanism of CF2Cl2 in CsNaY zeolite by using grand canonical Monte Carlo (GCMC) method. The accurate distribution of Al3+, Cs+, and Na+ in the CsNaY (Si/Al = 2.43) was obtained from molecular dynamics (MD) calculations and NMR simulation, while the potential parameters of the CF2Cl2 were determined by density functional theory (DFT) calculations. The experimental adsorption isotherm of the CF2Cl2 in the CsNaY was fully reproduced by the GCMC simulations. Furthermore, computer graphics (CG) visualization of the calculated results revealed the presence of two different mechanisms of CF2Cl2 adsorption in the CsNaY : (1) at low pressure, the CF2Cl2 selectively and drastically adsorbed at the Cs+ cations of the CsNaY : (2) at high pressure, the aggregation of the CF2Cl2 in the super cages of the CsNaY occurred. These results indicate that our new methodology, i. e. the combination of GCMC, MD, NMR simulation, DFT, and CG, is effective and useful not only to reproduce the experimental adsorption isotherm of chlorofluorocarbons in zeolites but also to clarify the atomistic mechanism of the adsorption, which cannot be obtained experimentally.
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U2 - 10.1016/s0167-2991(97)80647-7
DO - 10.1016/s0167-2991(97)80647-7
M3 - Article
AN - SCOPUS:0040765204
VL - 105 C
SP - 1811
EP - 1818
JO - Studies in Surface Science and Catalysis
JF - Studies in Surface Science and Catalysis
SN - 0167-2991
ER -