Potential model development using quantum chemical information for molecular simulation of adsorption equilibria of water-methanol (ethanol) mixtures in zeolite naa-4

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Abstract

A theoretical examination of two simple Lennard-Jones + Coulomb type potential models of zeolite NaA-4 was performed by quantum chemical calculations using density functional theory. A comparison of potential curves obtained from model parameters with those from quantum chemical calculations as a function of the position of a Na+ ion with respect to an appropriately chosen fragment of zeolite was used as a primary indicator in testing how realistic the behavior of the applied models is. This comparison provides a good starting point for further parameter tuning of a potential model using experimental data. The potential models were tested in different aspects: structural and adsorption equilibrium properties (quantum chemical structures vs pair correlation functions as well as equilibrium amount of adsorption) were calculated with pure water, methanol, and ethanol. Tuning the potential parameters resulted in a new model that satisfactorily reproduces the quantum chemical equilibrium location of the three adsorbates with respect to the zeolite framework. From the pair correlation functions, the behavior of the new potential model was found to be between those of the two investigated earlier models. Monte Carlo simulation of adsorption for water-methanol and water-ethanol mixtures showed that, at higher pressures (above p) 1 kPa), the newer model predicts greater adsorption selectivity of water to alcohols than the earlier models, which fits to available membrane permeation experiments better.

Original languageEnglish
Pages (from-to)12225-12235
Number of pages11
JournalJournal of Physical Chemistry C
Volume113
Issue number28
DOIs
Publication statusPublished - Jul 16 2009

Fingerprint

Zeolites
Methanol
Ethanol
ethyl alcohol
methyl alcohol
Adsorption
adsorption
Water
water
simulation
Tuning
tuning
Adsorbates
Permeation
Density functional theory
chemical equilibrium
alcohols
Alcohols
examination
selectivity

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Electronic, Optical and Magnetic Materials
  • Surfaces, Coatings and Films
  • Energy(all)

Cite this

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title = "Potential model development using quantum chemical information for molecular simulation of adsorption equilibria of water-methanol (ethanol) mixtures in zeolite naa-4",
abstract = "A theoretical examination of two simple Lennard-Jones + Coulomb type potential models of zeolite NaA-4 was performed by quantum chemical calculations using density functional theory. A comparison of potential curves obtained from model parameters with those from quantum chemical calculations as a function of the position of a Na+ ion with respect to an appropriately chosen fragment of zeolite was used as a primary indicator in testing how realistic the behavior of the applied models is. This comparison provides a good starting point for further parameter tuning of a potential model using experimental data. The potential models were tested in different aspects: structural and adsorption equilibrium properties (quantum chemical structures vs pair correlation functions as well as equilibrium amount of adsorption) were calculated with pure water, methanol, and ethanol. Tuning the potential parameters resulted in a new model that satisfactorily reproduces the quantum chemical equilibrium location of the three adsorbates with respect to the zeolite framework. From the pair correlation functions, the behavior of the new potential model was found to be between those of the two investigated earlier models. Monte Carlo simulation of adsorption for water-methanol and water-ethanol mixtures showed that, at higher pressures (above p) 1 kPa), the newer model predicts greater adsorption selectivity of water to alcohols than the earlier models, which fits to available membrane permeation experiments better.",
author = "{\'E}va Cs{\'a}nyi and Tam{\'a}s Krist{\'o}f and Gy{\"o}rgy Lendvay",
year = "2009",
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T1 - Potential model development using quantum chemical information for molecular simulation of adsorption equilibria of water-methanol (ethanol) mixtures in zeolite naa-4

AU - Csányi, Éva

AU - Kristóf, Tamás

AU - Lendvay, György

PY - 2009/7/16

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N2 - A theoretical examination of two simple Lennard-Jones + Coulomb type potential models of zeolite NaA-4 was performed by quantum chemical calculations using density functional theory. A comparison of potential curves obtained from model parameters with those from quantum chemical calculations as a function of the position of a Na+ ion with respect to an appropriately chosen fragment of zeolite was used as a primary indicator in testing how realistic the behavior of the applied models is. This comparison provides a good starting point for further parameter tuning of a potential model using experimental data. The potential models were tested in different aspects: structural and adsorption equilibrium properties (quantum chemical structures vs pair correlation functions as well as equilibrium amount of adsorption) were calculated with pure water, methanol, and ethanol. Tuning the potential parameters resulted in a new model that satisfactorily reproduces the quantum chemical equilibrium location of the three adsorbates with respect to the zeolite framework. From the pair correlation functions, the behavior of the new potential model was found to be between those of the two investigated earlier models. Monte Carlo simulation of adsorption for water-methanol and water-ethanol mixtures showed that, at higher pressures (above p) 1 kPa), the newer model predicts greater adsorption selectivity of water to alcohols than the earlier models, which fits to available membrane permeation experiments better.

AB - A theoretical examination of two simple Lennard-Jones + Coulomb type potential models of zeolite NaA-4 was performed by quantum chemical calculations using density functional theory. A comparison of potential curves obtained from model parameters with those from quantum chemical calculations as a function of the position of a Na+ ion with respect to an appropriately chosen fragment of zeolite was used as a primary indicator in testing how realistic the behavior of the applied models is. This comparison provides a good starting point for further parameter tuning of a potential model using experimental data. The potential models were tested in different aspects: structural and adsorption equilibrium properties (quantum chemical structures vs pair correlation functions as well as equilibrium amount of adsorption) were calculated with pure water, methanol, and ethanol. Tuning the potential parameters resulted in a new model that satisfactorily reproduces the quantum chemical equilibrium location of the three adsorbates with respect to the zeolite framework. From the pair correlation functions, the behavior of the new potential model was found to be between those of the two investigated earlier models. Monte Carlo simulation of adsorption for water-methanol and water-ethanol mixtures showed that, at higher pressures (above p) 1 kPa), the newer model predicts greater adsorption selectivity of water to alcohols than the earlier models, which fits to available membrane permeation experiments better.

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