Citation: WANG Yong-li, WU Bao-shan, HUO Chun-fang, TAO Zhi-chao, LI Yong-wang. A theoretical study on the adsorption of C_2~6 olefins on the H-ZSM-5 zeolite of periodic model[J]. Journal of Fuel Chemistry and Technology, ;2014, 42(8): 1001-1009. shu

A theoretical study on the adsorption of C_2~6 olefins on the H-ZSM-5 zeolite of periodic model

WANG Yong-li ^1,2 ,
WU Bao-shan ^1,3,, ,
HUO Chun-fang ^1,3 ,
TAO Zhi-chao ³ ,
LI Yong-wang ^1,3

1.
1. State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China;

Corresponding author: WU Bao-shan,
Received Date: 4 April 2014
Available Online: 13 June 2014
Fund Project: 国家重点基础研究发展规划(973计划,2011CB201401) (973计划,2011CB201401)中国科学院知识创新工程项目(KJCX2-YW-N41)。 (KJCX2-YW-N41)

The adsorption behaviors of linear C_2~6 olefins and butene isomers on the H-ZSM-5 zeolite of periodic model were studied by the PBE-D method. The adsorption energies (EPBE-D) and the dispersive correction energies (E_D) of C_2~6 linear olefins on the zeolite exhibit a linear increase with the number of carbons by -12 kJ/mol and -13 kJ/mol, respectively. The adsorption energies without dispersive correction (E^*) is not changed obviously, but it is decreased in the cases of increased space resistance for pentene and hexane. The value of E_D is much larger than that of E^*, implying that van der Waals' force plays a key role in the adsorption of olefins on the zeolite and its influence on the adsorption is dependent on the carbon number. The adsorption energies of butene isomers decrease in the order of trans-2-butane > cis-2-butene > n-butene > isobutene. Three kinds of n-butene isomers are similar in their E_D value, which are larger than that of n-butene. The difference in adsorption energy among the three isomers is caused by E^*. The differential charge density analysis shows that the electrons between the alkene double bond and the acidic center are gathered, in consistent with the strength of π-coordination; H atom in the acid site turns to be protonated, with electrons transferred to the nearby O and other atoms.
- adsorption of olefins,
- zeolite,
- periodic model,
- PBE-D,
- differential charge density
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沈阳化工大学材料科学与工程学院沈阳 110142

A theoretical study on the adsorption of C2~6 olefins on the H-ZSM-5 zeolite of periodic model

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通讯作者: 陈斌, bchen63@163.com

A theoretical study on the adsorption of C_2~6 olefins on the H-ZSM-5 zeolite of periodic model