A computational study of the adsorption of n-perfluorohexane in zeolite BCR-704

Peng Bai; Pritha Ghosh; Jeffrey C. Sung; Daniela Kohen; J. Ilja Siepmann; Randall Q. Snurr

doi:10.1016/j.fluid.2013.07.018

A computational study of the adsorption of n-perfluorohexane in zeolite BCR-704

Peng Bai, Pritha Ghosh, Jeffrey C. Sung, Daniela Kohen, J. Ilja Siepmann, Randall Q. Snurr

Research output: Contribution to journal › Article › peer-review

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Abstract

Monte Carlo simulations in the grand canonical and Gibbs ensembles were carried out to predict the adsorption isotherms of argon, nitrogen, and n-perfluorohexane in BCR-704, a faujasite-type calcium aluminosilicate with a Si/Al ratio of 1.6. Starting from existing force fields for the sorbate molecules and a transferable force field for all-silica zeolites, attempts were made to develop a force field that would reproduce the experimentally determined argon and nitrogen adsorption isotherms in BCR-704. However, good agreement for the nitrogen adsorption isotherm could only be obtained either for a set of force field parameters with a greatly reduced partial charge on the calcium cation or using a larger partial charge and assuming that co-adsorbed water molecules are present at the temperature used for the argon and nitrogen adsorption isotherms. Predictions of the adsorption isotherm for n-perfluorohexane in BCR-704 using the latter force field parameters and the FAU-X structure with a water/calcium ratio of 1 yield good agreement with the experimental benchmark data.

Original language	English (US)
Pages (from-to)	146-151
Number of pages	6
Journal	Fluid Phase Equilibria
Volume	366
DOIs	https://doi.org/10.1016/j.fluid.2013.07.018
State	Published - Mar 25 2014

Bibliographical note

Funding Information:
Financial support from the National Science Foundation ( CBET-1159837 for the development of the TraPPE-zeo force field and part of the initial simulations carried out at the University of Minnesota), the Defense Threat Reduction Agency ( HDTRA1-10-1-0023 for research at Northwestern University), the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences under Award DE-FG02-12ER16362 (for research at the University of Minnesota and Northwestern University enabling the longer simulations), and a graduate School Fellowship (P.B.) is gratefully acknowledged. Part of the computer resources was provided by the Minnesota Supercomputing Institute.

Keywords

Adsorption isotherm
Monte Carlo simulation
Zeolite

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10.1016/j.fluid.2013.07.018

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title = "A computational study of the adsorption of n-perfluorohexane in zeolite BCR-704",

abstract = "Monte Carlo simulations in the grand canonical and Gibbs ensembles were carried out to predict the adsorption isotherms of argon, nitrogen, and n-perfluorohexane in BCR-704, a faujasite-type calcium aluminosilicate with a Si/Al ratio of 1.6. Starting from existing force fields for the sorbate molecules and a transferable force field for all-silica zeolites, attempts were made to develop a force field that would reproduce the experimentally determined argon and nitrogen adsorption isotherms in BCR-704. However, good agreement for the nitrogen adsorption isotherm could only be obtained either for a set of force field parameters with a greatly reduced partial charge on the calcium cation or using a larger partial charge and assuming that co-adsorbed water molecules are present at the temperature used for the argon and nitrogen adsorption isotherms. Predictions of the adsorption isotherm for n-perfluorohexane in BCR-704 using the latter force field parameters and the FAU-X structure with a water/calcium ratio of 1 yield good agreement with the experimental benchmark data.",

keywords = "Adsorption isotherm, Monte Carlo simulation, Zeolite",

author = "Peng Bai and Pritha Ghosh and Sung, {Jeffrey C.} and Daniela Kohen and Siepmann, {J. Ilja} and Snurr, {Randall Q.}",

note = "Funding Information: Financial support from the National Science Foundation ( CBET-1159837 for the development of the TraPPE-zeo force field and part of the initial simulations carried out at the University of Minnesota), the Defense Threat Reduction Agency ( HDTRA1-10-1-0023 for research at Northwestern University), the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences under Award DE-FG02-12ER16362 (for research at the University of Minnesota and Northwestern University enabling the longer simulations), and a graduate School Fellowship (P.B.) is gratefully acknowledged. Part of the computer resources was provided by the Minnesota Supercomputing Institute.",

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AU - Snurr, Randall Q.

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N2 - Monte Carlo simulations in the grand canonical and Gibbs ensembles were carried out to predict the adsorption isotherms of argon, nitrogen, and n-perfluorohexane in BCR-704, a faujasite-type calcium aluminosilicate with a Si/Al ratio of 1.6. Starting from existing force fields for the sorbate molecules and a transferable force field for all-silica zeolites, attempts were made to develop a force field that would reproduce the experimentally determined argon and nitrogen adsorption isotherms in BCR-704. However, good agreement for the nitrogen adsorption isotherm could only be obtained either for a set of force field parameters with a greatly reduced partial charge on the calcium cation or using a larger partial charge and assuming that co-adsorbed water molecules are present at the temperature used for the argon and nitrogen adsorption isotherms. Predictions of the adsorption isotherm for n-perfluorohexane in BCR-704 using the latter force field parameters and the FAU-X structure with a water/calcium ratio of 1 yield good agreement with the experimental benchmark data.

AB - Monte Carlo simulations in the grand canonical and Gibbs ensembles were carried out to predict the adsorption isotherms of argon, nitrogen, and n-perfluorohexane in BCR-704, a faujasite-type calcium aluminosilicate with a Si/Al ratio of 1.6. Starting from existing force fields for the sorbate molecules and a transferable force field for all-silica zeolites, attempts were made to develop a force field that would reproduce the experimentally determined argon and nitrogen adsorption isotherms in BCR-704. However, good agreement for the nitrogen adsorption isotherm could only be obtained either for a set of force field parameters with a greatly reduced partial charge on the calcium cation or using a larger partial charge and assuming that co-adsorbed water molecules are present at the temperature used for the argon and nitrogen adsorption isotherms. Predictions of the adsorption isotherm for n-perfluorohexane in BCR-704 using the latter force field parameters and the FAU-X structure with a water/calcium ratio of 1 yield good agreement with the experimental benchmark data.

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A computational study of the adsorption of n-perfluorohexane in zeolite BCR-704

Abstract

Bibliographical note

Keywords

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NMGC: Nanoporous Materials Genome: Methods and Software to Optimize Gas Storage, Separations, and Catalysis (Phase 1)

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A computational study of the adsorption of n-perfluorohexane in zeolite BCR-704

Abstract

Bibliographical note

Keywords

Access

OpenUrl availability

Other files and links

Fingerprint

Projects

NMGC: Nanoporous Materials Genome: Methods and Software to Optimize Gas Storage, Separations, and Catalysis (Phase 1)

Cite this