Chem. J. Chinese Universities

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Structure, Acid Properties and Catalysis Performance of Dealuminated MCM-49 Zeolites for the Alkylation of Benzene with Propylene

ZHANG Yu1,2, WU Shu-Jie1, YANG Xu-Wei1, JIA Ming-Jun1, WANG Li-Xia1, ZHANG Zuo-Wang1, WU Tong-Hao1*, SUN Chia-Chong3   

    1. Department of Physical Chemistry, College of Chemistry, Jilin University, Changchun 130022, China;
    2. Department of Chemical Engineering, Jilin Institute of Chemical Technology, Jilin 132022, China;
    3. National Key Laboratory of Theoretical and Computational Chemistry, Jilin Univrsity, Changchun 130021, China
  • Received:2006-12-12 Revised:1900-01-01 Online:2007-07-10 Published:2007-07-10
  • Contact: WU Tong-Hao

Abstract:

Nano MCM-49 zeolite was synthesized and dealuminated by acid reflux and hydrothermal treatment, respectively. The resulting solids were characterized via XRD, N2 adsorption-desorption, NH3-TPD, FTIR and 27Al NMR. The amounts of total acid sites on dealuminated MCM-49 samples were decreased. For the acid reflux samples, the acid strength is not modified. For the hydrothermally dealuminated zeolite at 600 ℃, the acid strength is weaker as observed by NH3-TPD studies. 27Al NMR reveals that the acid dealumination at room temperature for 5 h results in a decrease of the amounts of aluminum atoms in framework of zeolite. After dealumination under acid reflux for 10 h, the spectrum becomes broader, and the shape of the peak corresponding to the tetrahedral aluminum atoms was modified. After hydrothermal dealumination at 600 ℃ for 3 h the broadening of the peaks increased and a new peak at δ 30 appeared, due to extraframework aluminum in a tetra- or pentacoordinate. Nano MCM-49 zeolite shows an excellent catalytic activity and selectivity in the liquid-phase alkylation of benzene with propylene. The conversion of propylene reaches 99.5%, and the selectivity to IPB is 73.6%. The propylene conversion can be decreased by dealumination. Comparision of the product distribution between MCM-49 and dealuminated MCM-49 suggests that dealumination could improve the selectivity to monoalkylation. For D-25-5 zeolite, the conversion of propylene is parallel to that of MCM-49 zeolite, while the yield to IPB increases 5.3%.

Key words: Dealuminated MCM-49 zeolite, Alkylation, Catalysis performance

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