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多级孔ZSM-5分子筛的制备及其催化甲醇芳构化反应性能
引用本文:杨秀娜,姜阳,齐慧敏.多级孔ZSM-5分子筛的制备及其催化甲醇芳构化反应性能[J].化工进展,2016,35(11):3536-3541.
作者姓名:杨秀娜  姜阳  齐慧敏
作者单位:中国石油化工股份有限公司抚顺石油化工研究院, 辽宁 抚顺 113001
基金项目:中国石油化工集团公司项目(115086)。
摘    要:采用晶种法,在合成体系中引入十六烷基三甲基溴化铵(CTAB)制备了具有多级孔道的ZSM-5分子筛。采用XRD、SEM、NH3-TPD、XRF和氮气吸附等多种技术对其进行了表征,并考察了不同CTAB添加量对该分子筛结构、酸性及其在甲醇芳构化反应中催化性能的影响。结果表明,CTAB的添加显著影响分子筛的形貌、孔结构及分子筛的酸性,进而决定其在甲醇制芳烃反应中的稳定性和芳构化选择性。分子筛增加的介孔性提高了大分子化合物的扩散,进而提高了催化剂寿命。CTAB的添加抑制了铝源进入骨架进行配位,增加CTAB的用量导致Si/Al比提高,进而导致分子筛酸性下降以及芳烃选择性下降。

关 键 词:甲醇芳构化  ZSM-5分子筛  多级孔  催化剂寿命  
收稿时间:2016-03-04

Synthesis of hierarchical ZSM-5 molecular sieves and evaluation of their catalytic performance in methanol aromatization
YANG Xiuna,JIANG Yang,QI Huimin.Synthesis of hierarchical ZSM-5 molecular sieves and evaluation of their catalytic performance in methanol aromatization[J].Chemical Industry and Engineering Progress,2016,35(11):3536-3541.
Authors:YANG Xiuna  JIANG Yang  QI Huimin
Affiliation:Fushun Research Institute of Petroleum and Petrochemicals, SINOPEC, Fushun 113001, Liaoning, China
Abstract:A series of ZSM-5 nanozeolites with hierarchical porosity were prepared by a seeding method of adding cetyltrimethyl ammonium bromide (CTAB). The hierarchical ZSM-5 molecular sieves were characterized by XRD, SEM, NH3-TPD, XRF and N2 sorption. The impacts of CTAB amount on the zeolite structure, acid property and the catalytic performance in methanol aromatization were investigated. The results indicated that the CTAB amount significantly affected the crystal morphology, pore structure, acidity and thus influenced the catalytic stability and aromatic selectivity considerably. The hierarchical ZSM-5 catalysts exhibited an increased mesopores by introducing CTAB and high stability for the MTA reaction due to the enhanced mass transfer and reduced diffusion limitation. Also, the formation of framework Al was suppressed by the addition of CTAB. The Si/Al ratio was increased by increasing the amounts of CTAB, which decreased the acidity of hierarchical ZSM-5 molecular sieves and the aromatics selectivity.
Keywords:methanol aromatization  ZSM-5 molecular sieves  hierarchical  catalyst lifetime  
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