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ISSN 1000-6818CN 11-1892/O6CODEN WHXUEU
Acta Phys Chim Sin >> 2012,Vol.28>> Issue(07)>> 1630-1636     doi: 10.3866/PKU.WHXB201204171         中文摘要
THEORETICAL AND COMPUTATIONAL CHEMISTRY
Theoretical Study on the Synthesis of Ethyl Tertiary Butyl Ether over HZSM-5 Zeolite
LI Jun-Nan, PU Min, SU Yong, HE Jing, EVANS David G.
State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, P. R. China
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The formation mechanism of ethyl tertiary butyl ether (ETBE) from ethanol and isobutene catalyzed by HZSM-5 has been investigated using the ONIOM (B3LYP/6-31G(d,p):UFF) method. The calculation results of the reactants adsorbability reveal that the interaction between ethanol and the acidic sites on HZSM-5 leads to the formation of hydrogen bonds. The interaction between isobutene and Brönsted acidic sites leads to the formation of a π-complex. It is subsequently found that the mechanism of the ETBE formation from ethanol and isobutene catalyzed by HZSM-5 is a concerted reaction, and that the order of reactant adsorption onto HZSM-5 affected the reaction. The favorable pathway is based on the complex formed by the simultaneous adsorption of ethanol and isobutene, in which the H atom of the π-complex is transferred to the C atom of the C=C in isobutene, and the O atom of the adsorbed ethanol is transferred to the other C atom of the C=C to form the C-O bond. In this process, the proton of the acidic sites adds to the C=C bond forming the C-H bond, and the H atom of the ethanol hydroxyl interacts with acidic sites, generating a new proton. The corresponding lowest energy barrier was 25.14 kJ·mol-1.



Keywords: Ethanol   Isobutene   HZSM-5 zeolite   ONIOM   Ethyl tertiary butyl ether  
Received: 2011-12-01 Accepted: 2012-03-26 Publication Date (Web): 2012-04-17
Corresponding Authors: PU Min Email: pumin@mail.buct.edu.cn


Cite this article: LI Jun-Nan, PU Min, SU Yong, HE Jing, EVANS David G.. Theoretical Study on the Synthesis of Ethyl Tertiary Butyl Ether over HZSM-5 Zeolite[J]. Acta Phys. -Chim. Sin., 2012,28 (07): 1630-1636.    doi: 10.3866/PKU.WHXB201204171

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