How does benzene in NaY zeolite couple to the framework vibrations?

F. Jousse, D.P. Vercauteren, S.M. Auerbach

Research output: Contribution to journalArticle

Abstract

Constrained energy minimization, equilibrium and nonequilibrium molecular dynamics calculations, and constrained Monte Carlo simulations were used to determine the influence of the coupling between benzene adsorbed in a NaY zeolite model (Si/Al = 2) and the framework vibrations on benzene site-to-site dynamics. Benzene at an S site is strongly coupled to the nearby Na(II) cation, resulting in a decrease of the external vibrational frequency of the center-of-mass of benzene away from this cation by 60 cm. Despite this coupling, framework vibrations have remarkably little influence on the site-to-site rate constants of benzene. Although with a fixed framework no dissipation of the excess kinetic energy of the adsorbed molecule can take place and thus no thermalization to equilibrium, energy redistribution from the translational motion of benzene into the internal degrees of freedom of the flexible molecule is seen to provide a good thermalization.
Original languageEnglish
Pages (from-to)8768-8778
Number of pages11
JournalJournal of physical chemistry B
Volume104
DOIs
Publication statusPublished - 1 Sep 2000

Fingerprint

Benzene
Positive ions
Molecules
Vibrational spectra
Kinetic energy
Molecular dynamics
Rate constants

Cite this

@article{bdd92f5b74cc412bae77d783c01ce46d,
title = "How does benzene in NaY zeolite couple to the framework vibrations?",
abstract = "Constrained energy minimization, equilibrium and nonequilibrium molecular dynamics calculations, and constrained Monte Carlo simulations were used to determine the influence of the coupling between benzene adsorbed in a NaY zeolite model (Si/Al = 2) and the framework vibrations on benzene site-to-site dynamics. Benzene at an S site is strongly coupled to the nearby Na(II) cation, resulting in a decrease of the external vibrational frequency of the center-of-mass of benzene away from this cation by 60 cm. Despite this coupling, framework vibrations have remarkably little influence on the site-to-site rate constants of benzene. Although with a fixed framework no dissipation of the excess kinetic energy of the adsorbed molecule can take place and thus no thermalization to equilibrium, energy redistribution from the translational motion of benzene into the internal degrees of freedom of the flexible molecule is seen to provide a good thermalization.",
author = "F. Jousse and D.P. Vercauteren and S.M. Auerbach",
note = "Copyright 2004 Elsevier Science B.V., Amsterdam. All rights reserved.",
year = "2000",
month = "9",
day = "1",
doi = "10.1021/jp9942872",
language = "English",
volume = "104",
pages = "8768--8778",
journal = "Journal of physical chemistry B",
issn = "1089-5647",
publisher = "American Chemical Society",

}

How does benzene in NaY zeolite couple to the framework vibrations? / Jousse, F.; Vercauteren, D.P.; Auerbach, S.M.

In: Journal of physical chemistry B, Vol. 104, 01.09.2000, p. 8768-8778.

Research output: Contribution to journalArticle

TY - JOUR

T1 - How does benzene in NaY zeolite couple to the framework vibrations?

AU - Jousse, F.

AU - Vercauteren, D.P.

AU - Auerbach, S.M.

N1 - Copyright 2004 Elsevier Science B.V., Amsterdam. All rights reserved.

PY - 2000/9/1

Y1 - 2000/9/1

N2 - Constrained energy minimization, equilibrium and nonequilibrium molecular dynamics calculations, and constrained Monte Carlo simulations were used to determine the influence of the coupling between benzene adsorbed in a NaY zeolite model (Si/Al = 2) and the framework vibrations on benzene site-to-site dynamics. Benzene at an S site is strongly coupled to the nearby Na(II) cation, resulting in a decrease of the external vibrational frequency of the center-of-mass of benzene away from this cation by 60 cm. Despite this coupling, framework vibrations have remarkably little influence on the site-to-site rate constants of benzene. Although with a fixed framework no dissipation of the excess kinetic energy of the adsorbed molecule can take place and thus no thermalization to equilibrium, energy redistribution from the translational motion of benzene into the internal degrees of freedom of the flexible molecule is seen to provide a good thermalization.

AB - Constrained energy minimization, equilibrium and nonequilibrium molecular dynamics calculations, and constrained Monte Carlo simulations were used to determine the influence of the coupling between benzene adsorbed in a NaY zeolite model (Si/Al = 2) and the framework vibrations on benzene site-to-site dynamics. Benzene at an S site is strongly coupled to the nearby Na(II) cation, resulting in a decrease of the external vibrational frequency of the center-of-mass of benzene away from this cation by 60 cm. Despite this coupling, framework vibrations have remarkably little influence on the site-to-site rate constants of benzene. Although with a fixed framework no dissipation of the excess kinetic energy of the adsorbed molecule can take place and thus no thermalization to equilibrium, energy redistribution from the translational motion of benzene into the internal degrees of freedom of the flexible molecule is seen to provide a good thermalization.

UR - http://www.scopus.com/inward/record.url?scp=0034257963&partnerID=8YFLogxK

U2 - 10.1021/jp9942872

DO - 10.1021/jp9942872

M3 - Article

VL - 104

SP - 8768

EP - 8778

JO - Journal of physical chemistry B

JF - Journal of physical chemistry B

SN - 1089-5647

ER -