Effect of topology and molecular occupancy on self-diffusion in lattice models of zeolites - Monte-Carlo simulations

Marc Olivier Coppens; Alexis T. Bell; Arup K. Chakraborty

doi:10.1016/s0009-2509(98)00047-5

Effect of topology and molecular occupancy on self-diffusion in lattice models of zeolites - Monte-Carlo simulations

Marc Olivier Coppens, Alexis T. Bell, Arup K. Chakraborty

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

72 Scopus citations

Abstract

The dependence of hopping diffusion on lattice topology and occupancy by the diffusing molecules is studied using Monte-Carlo simulations. For poorly connected lattices, such as ZSM-5/silicalite, the self-diffusivity deviates strongly from the linear mean-field result, especially at high occupancies. A time-correlation formalism is derived to predict these deviations which are proportional to the accumulated correlation between the displacement at some time and the first attempted hop. Renormalized deviations depend on lattice topology, but not on occupancy, so that the curves for various occupancies can be collapsed on to a single curve which can be well approximated by a stretched exponential. The results show that a mean-field theory with correlated time steps should work adequately for well-connected lattices, but poor performance is predicted for such poorly connected lattices as ZSM-5.

Original language	English
Pages (from-to)	2053-2061
Number of pages	9
Journal	Chemical Engineering Science
Volume	53
Issue number	11
DOIs	https://doi.org/10.1016/s0009-2509(98)00047-5
State	Published - 1 Jun 1998
Externally published	Yes

Bibliographical note

Funding Information:
This work was supported by the Office of Industrial Technology of the U.S. Department of Energy under contract DE-AC03-SF7600098. A Fellowship from the Belgian American Educational Foundation, a Fellowship as an “Aspirant” from the F.W.O. (Fund for Scientific Research–Flanders, Belgium) and a F.W.O.–N.S.F. grant for the first stages of this project are gratefully acknowledged. Continued funding of this project was provided by a Postdoctoral Fellowship from the Fund for Scientific Research–Flanders, Belgium (F.W.O.)

Funding

This work was supported by the Office of Industrial Technology of the U.S. Department of Energy under contract DE-AC03-SF7600098. A Fellowship from the Belgian American Educational Foundation, a Fellowship as an “Aspirant” from the F.W.O. (Fund for Scientific Research–Flanders, Belgium) and a F.W.O.–N.S.F. grant for the first stages of this project are gratefully acknowledged. Continued funding of this project was provided by a Postdoctoral Fellowship from the Fund for Scientific Research–Flanders, Belgium (F.W.O.)

Funders	Funder number
F.W.O.
Fund for Scientific Research–Flanders, Belgium
Office of Industrial Technology
U.S. Department of Energy	DE-AC03-SF7600098
Belgian American Educational Foundation

Keywords

Diffusion
Monte-Carlo
Zeolites

Access to Document

10.1016/s0009-2509(98)00047-5

Cite this

@article{133df35c5d634a83b588a33313cfd1d7,

title = "Effect of topology and molecular occupancy on self-diffusion in lattice models of zeolites - Monte-Carlo simulations",

abstract = "The dependence of hopping diffusion on lattice topology and occupancy by the diffusing molecules is studied using Monte-Carlo simulations. For poorly connected lattices, such as ZSM-5/silicalite, the self-diffusivity deviates strongly from the linear mean-field result, especially at high occupancies. A time-correlation formalism is derived to predict these deviations which are proportional to the accumulated correlation between the displacement at some time and the first attempted hop. Renormalized deviations depend on lattice topology, but not on occupancy, so that the curves for various occupancies can be collapsed on to a single curve which can be well approximated by a stretched exponential. The results show that a mean-field theory with correlated time steps should work adequately for well-connected lattices, but poor performance is predicted for such poorly connected lattices as ZSM-5.",

keywords = "Diffusion, Monte-Carlo, Zeolites",

author = "Coppens, {Marc Olivier} and Bell, {Alexis T.} and Chakraborty, {Arup K.}",

note = "Funding Information: This work was supported by the Office of Industrial Technology of the U.S. Department of Energy under contract DE-AC03-SF7600098. A Fellowship from the Belgian American Educational Foundation, a Fellowship as an “Aspirant” from the F.W.O. (Fund for Scientific Research–Flanders, Belgium) and a F.W.O.–N.S.F. grant for the first stages of this project are gratefully acknowledged. Continued funding of this project was provided by a Postdoctoral Fellowship from the Fund for Scientific Research–Flanders, Belgium (F.W.O.)",

year = "1998",

month = jun,

day = "1",

doi = "10.1016/s0009-2509(98)00047-5",

language = "אנגלית",

volume = "53",

pages = "2053--2061",

journal = "Chemical Engineering Science",

issn = "0009-2509",

publisher = "Elsevier BV",

number = "11",

}

TY - JOUR

T1 - Effect of topology and molecular occupancy on self-diffusion in lattice models of zeolites - Monte-Carlo simulations

AU - Coppens, Marc Olivier

AU - Bell, Alexis T.

AU - Chakraborty, Arup K.

N1 - Funding Information: This work was supported by the Office of Industrial Technology of the U.S. Department of Energy under contract DE-AC03-SF7600098. A Fellowship from the Belgian American Educational Foundation, a Fellowship as an “Aspirant” from the F.W.O. (Fund for Scientific Research–Flanders, Belgium) and a F.W.O.–N.S.F. grant for the first stages of this project are gratefully acknowledged. Continued funding of this project was provided by a Postdoctoral Fellowship from the Fund for Scientific Research–Flanders, Belgium (F.W.O.)

PY - 1998/6/1

Y1 - 1998/6/1

N2 - The dependence of hopping diffusion on lattice topology and occupancy by the diffusing molecules is studied using Monte-Carlo simulations. For poorly connected lattices, such as ZSM-5/silicalite, the self-diffusivity deviates strongly from the linear mean-field result, especially at high occupancies. A time-correlation formalism is derived to predict these deviations which are proportional to the accumulated correlation between the displacement at some time and the first attempted hop. Renormalized deviations depend on lattice topology, but not on occupancy, so that the curves for various occupancies can be collapsed on to a single curve which can be well approximated by a stretched exponential. The results show that a mean-field theory with correlated time steps should work adequately for well-connected lattices, but poor performance is predicted for such poorly connected lattices as ZSM-5.

AB - The dependence of hopping diffusion on lattice topology and occupancy by the diffusing molecules is studied using Monte-Carlo simulations. For poorly connected lattices, such as ZSM-5/silicalite, the self-diffusivity deviates strongly from the linear mean-field result, especially at high occupancies. A time-correlation formalism is derived to predict these deviations which are proportional to the accumulated correlation between the displacement at some time and the first attempted hop. Renormalized deviations depend on lattice topology, but not on occupancy, so that the curves for various occupancies can be collapsed on to a single curve which can be well approximated by a stretched exponential. The results show that a mean-field theory with correlated time steps should work adequately for well-connected lattices, but poor performance is predicted for such poorly connected lattices as ZSM-5.

KW - Diffusion

KW - Monte-Carlo

KW - Zeolites

UR - http://www.scopus.com/inward/record.url?scp=0032511198&partnerID=8YFLogxK

U2 - 10.1016/s0009-2509(98)00047-5

DO - 10.1016/s0009-2509(98)00047-5

M3 - ???researchoutput.researchoutputtypes.contributiontojournal.article???

AN - SCOPUS:0032511198

SN - 0009-2509

VL - 53

SP - 2053

EP - 2061

JO - Chemical Engineering Science

JF - Chemical Engineering Science

IS - 11

ER -

Effect of topology and molecular occupancy on self-diffusion in lattice models of zeolites - Monte-Carlo simulations

Abstract

Bibliographical note

Funding

Keywords

Access to Document

Other files and links

Fingerprint

Cite this