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Preparation of Fe/ZSM-5 and catalytic behavior for toluene alkylation with methanol

ZHANG Lidong,GAO Junhua,HU Jinxian,LI Wenhuai,WANG Jianguo   

  1. State Key Laboratory of Coal Conversion,Institute of Coal Chemistry,Chinese Academy of Sciences;Graduate University of the Chinese Academy of Sciences
  • Online:2009-08-05 Published:2009-08-05

Fe/ZSM-5的制备及其催化甲苯/甲醇烷基化反应行为

张立东,高俊华,胡津仙,李文怀,王建国   

  1. 中国科学院山西煤炭化学研究所煤转化国家重点实验室;中国科学院研究生院

Abstract: A series of Fe/ZSM-5 zeolites with different contents of Fe were hydrothermally synthesized by changing the Si/Fe ratio (the same gel of SiO2/Al2O3=100) and their catalytic performance for toluene alkylation with methanol was investigated in a continuous fluid fixed bed reactor at normal atmosphere. The structure, pore properties and acidity of Fe/ZSM-5 zeolites were characterized by X-ray diffraction, electronic paramagnet resonance, low temperature N2 adsorption, NH3-TPD and Py-IR. The results indicate that the partial introduction of Fe atoms into the zeolite frameworks in the synthetic process does not destroy the ZSM-5 framework structure, while it leads to the decrease in crystallization capacity, the change in acidity and the lowering in the acid strength. As a result, the coke formation during the alkylation reaction process is suppressed. Hence, the stability of zeolite and the utilization ratio of methanol are improved.

摘要: 采用水热晶化的方法,通过改变凝胶Si/Fe比例合成了一系列不同铁含量的Fe/ZSM-5分子筛(凝胶投料硅铝比为100)。在常压连续流动固定床反应器上,考察了Fe/ZSM-5分子筛用于催化甲苯甲醇烷基化的反应行为。采用X射线衍射、电子顺磁共振、N2物理吸附、氨程序升温脱附及吡啶吸附红外光谱等方法研究了Fe/ZSM-5分子筛的结构及孔结构性质和酸性。实验结果表明,在合成过程中引入铁原子,使部分铁原子进入分子筛骨架,并没有破坏ZSM-5分子筛的骨架结构,但降低了分子筛结晶度,改变了分子筛酸性质,降低了分子筛酸强度;Fe/ZSM-5抑制了积炭的形成,分子筛稳定性以及甲醇烷基化利用率得到明显提高。

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