Molecular Simulations of Adsorption and Diffusion Behaviors of Benzene Molecules in NaY Zeolite

CIESC Journal ›› 2009, Vol. 17 ›› Issue (4): 618-624.

Molecular Simulations of Adsorption and Diffusion Behaviors of Benzene Molecules in NaY Zeolite

张舟¹, 刘辉¹, 朱吉钦¹, 陈标华¹, 田辉平², 贺振富²

1. State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China;
2. Research Institute of Petroleum Processing, SINOPEC, Beijing 100083, China

收稿日期:2008-11-20 修回日期:2009-06-04 出版日期:2009-08-28 发布日期:2010-12-30
通讯作者: LIU Hui, E-mail: hliu@mail.buct.edu.cn
作者简介:
基金资助:
Supported by the State Key Development Program for Basic Research of China(2004CB719505);the National Natural Science Foundation of China(20625621)

Molecular Simulations of Adsorption and Diffusion Behaviors of Benzene Molecules in NaY Zeolite

ZHANG Zhou¹, LIU Hui¹, ZHU Jiqin¹, CHEN Biaohua¹, TIAN Huiping², HE Zhenfu²

1. State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China;
2. Research Institute of Petroleum Processing, SINOPEC, Beijing 100083, China

Received:2008-11-20 Revised:2009-06-04 Online:2009-08-28 Published:2010-12-30
Supported by:
Supported by the State Key Development Program for Basic Research of China(2004CB719505);the National Natural Science Foundation of China(20625621)

摘要/Abstract

摘要： In the article the Grand Canonical Monte Carlo(GCMC),molecular dynamics(MD),and kinetic Monte Carlo(KMC)simulations with particular focus on ascertaining the loading dependence of benzene diffusion in the zeolite were performed.First,a realistic representation of the structure of the sorbate-sorbent system was obtained based on GCMC simulation.The simulation clearly shows the characteristics of the adsorption sites of the benzene-NaY system,from which two kinds of preferably adsorbing sites for benzene molecules,called S_Ⅱ and W sites,are identified.The structure thus obtained was then used as a basis for KMC and MD simulations.A comparative study by introducing and comparing two different mechanisms underlying jump diffusion in the zeolite of interest shows that the MS diffusivity values predicted by the KMC and MD methods are fairly close to each other,leading to the conclusion that for benzene diffusion in NaY,the S_Ⅱ→W→S_Ⅱ jumps of benzene molecules are dominated,while the W→W jumps do not exist in the process.These findings provide further support to our previous conclusion about the absence of the W→W jumps in the process of benzene diffusion in NaY.Finally,two relations for predicting the self-and MS diffusivities were derived and found to be in fair agreement with the KMC and MD simulations.

关键词: benzene, adsorption, diffusion, NaY, Grand Canonical Monte Carlo, kinetic Monte Carlo

Abstract: In the article the Grand Canonical Monte Carlo(GCMC),molecular dynamics(MD),and kinetic Monte Carlo(KMC)simulations with particular focus on ascertaining the loading dependence of benzene diffusion in the zeolite were performed.First,a realistic representation of the structure of the sorbate-sorbent system was obtained based on GCMC simulation.The simulation clearly shows the characteristics of the adsorption sites of the benzene-NaY system,from which two kinds of preferably adsorbing sites for benzene molecules,called S_Ⅱ and W sites,are identified.The structure thus obtained was then used as a basis for KMC and MD simulations.A comparative study by introducing and comparing two different mechanisms underlying jump diffusion in the zeolite of interest shows that the MS diffusivity values predicted by the KMC and MD methods are fairly close to each other,leading to the conclusion that for benzene diffusion in NaY,the S_Ⅱ→W→S_Ⅱ jumps of benzene molecules are dominated,while the W→W jumps do not exist in the process.These findings provide further support to our previous conclusion about the absence of the W→W jumps in the process of benzene diffusion in NaY.Finally,two relations for predicting the self-and MS diffusivities were derived and found to be in fair agreement with the KMC and MD simulations.

Key words: benzene, adsorption, diffusion, NaY, Grand Canonical Monte Carlo, kinetic Monte Carlo

张舟, 刘辉, 朱吉钦, 陈标华, 田辉平, 贺振富. Molecular Simulations of Adsorption and Diffusion Behaviors of Benzene Molecules in NaY Zeolite[J]. CIESC Journal, 2009, 17(4): 618-624.

ZHANG Zhou, LIU Hui, ZHU Jiqin, CHEN Biaohua, TIAN Huiping, HE Zhenfu. Molecular Simulations of Adsorption and Diffusion Behaviors of Benzene Molecules in NaY Zeolite[J]. , 2009, 17(4): 618-624.

参考文献

1 Krishna,R.,“Diffusion of binary mixtures in zeolites:Molecular dynamics simulations versus Maxwell-Stefan theory”,Chemical Physics Letters,326,477-484(2000).
2 Namuangruk,S.,Pantu,P.,Limtrakul,J.,“Alkylation of benzene with ethylene over faujasite zeolite investigated by the ONIOMmethod”,Journal of Catalysis,225,523-530(2004).
3 Klein,H.,Kirschhock,C.,Fuess,H.,“Adsorption and diffusion of aromatic hydrocarbons in zeolite Y by molecular mechanics calculation and X-ray powder diffraction”,J.Phys.Chem.,98, 12345-12360(1994).
4 Auerbach,S.M.,Hensont,N.J.,Cheetham,A.K.,Metiu,H.I., “Transport theory for cationic zeolites:Diffusion of benzene in Na-Y”,J.Phys.Chem.,99,10600-10608(1995).
5 Bremard,C.,“Organometallic chemistry of group VI metals in the void space of zeolites”,Coordination Chemistry Reviews,178-180, 1647-1677(1998).
6 Auerbach,S.M.,Metiu,H.I.,“Diffusion in zeolites via cage-to-cage kinetics:Modeling benzene diffusion in Na-Y”,J.Chem.Phys.,105, 3753-3760(1996).
7 Paschek,D.,Krishna,R.,“Monte Carlo simulations of self-and transport-diffusivities of 2-methylhexane in silicalite”,Phys.Chem. Chem.Phys.,2,2389-2394(2000).
8 Saravanan,C.,Auerbacha,S.M.,“Modeling the loading dependence of diffusion in zeolites(I)Analytical theory for benzene in Na-Y”,J. Chem.Phys.,107(19),8120-8131(1997).
9 Saravanan,C.,Auerbacha,S.M.,“Modeling the loading dependence of diffusion in zeolites(II)Kinetic Monte Carlo simulations of benzene in Na-Y”,J.Chem.Phys.,107(19),8133-8137(1997).
10 Auerbach,S.M.,Horia,I.M.,“Diffusion in zeolites via cage-to-cage kinetics:Modeling benzene diffusion in Na-Y”,J.Chem.Phys.,105 (9),3753-3760(1996).
11 Zhang,Z.,Liu,H.,Chen,B.H.,“Self-diffusivity of benzene in zeolite Y:Different jump diffusion mechanisms investigated by KMC simulations”,J.Chem.Ind.Eng.(China),57(5),1147-1152(2006). (in Chinese)
12 Zhang,Z.,Liu,H.,Chen,B.H.,“occupancy dependence of M-S diffusivity of single component in MFI zeolite”,J.Chem.Ind.Eng. (China),56(11),2054-2058(2005).(in Chinese)
13 Bergerhoff,G.,Baur,W.H.,Nowacki,W.,“The crystal structure of faujasite”,Neues Jahrbuch fur Mineralogie,Monatshefte,193-200 (1958).
14 Olson,D.H.,“Crystal structure of the zeolite nickel faujasite”,J. Phys.Chem.,72,4366-4373(1968).
15 Fitch,A.N.,Jobic,H.,Renouprez,A.,“Localization of benzene in sodium-Y zeolite by powder neutron diffraction”,J.Phys.Chem.,90, 1311-1318(1986).
16 Klein,H.,Kirschhock,C.,Fuess,H.,“Adsorption and diffusion of aromatic hydrocarbons in zeolite Y by molecular mechanics calculation and X-ray powder diffraction”,J.Phys.Chem.,98,12345-12360 (1994).
17 Frenkel,S.,Understanding Molecular Simulation—From Algorithms to Applications,Academic Press,Amsterdam(1996).
18 Klein,H.,Fuess,H.,Schrimpf,G.,“Mobility of aromatic molecules in zeolite NaY by molecular dynamics simulation”,J.Phys.Chem., 100,11101-11112(1996).
19 Krishna,R.,Paschek,D.,“Verification of the Maxwell-Stefan theory for tracer diffusion in zeolites”,Chem.Eng.J.,85,7-15(2002).

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Molecular Simulations of Adsorption and Diffusion Behaviors of Benzene Molecules in NaY Zeolite

Molecular Simulations of Adsorption and Diffusion Behaviors of Benzene Molecules in NaY Zeolite

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