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孔壁含有沸石次级结构单元的MCM-48的合成及催化研究

Synthesis of mesoporous MCM-48 containing zeolite secondary building units and it′s catalytic properties

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【作者】 李强窦涛张瑛李玉平王姗孙发民

【Author】 LI Qiang~1,DOU Tao~(1,2),ZHANG Ying~1,LI Yu-Ping~2,WANG Shan~2,SUN Fa-Min~3(1.The CNPC Key Laboratory of Catalysis,China University of Petroleum(Beijing),Beijing 102249,China;2.Institute of Special Chemicals,Taiyuan University of Technology,Taiyuan 030024,China;3.Institute of Daqing Petro Chemical,Daqing 163714,China)

【机构】 中国石油大学(北京)化工学院CNPC催化重点实验室太原理工大学精细化工研究所大庆石化公司研究院 北京102249北京102249山西太原030024黑龙江大庆163714

【摘要】 以双表面活性剂(双极性头表面活性剂和三乙醇胺)为模板,以含有沸石次级结构单元的溶胶为前驱体,在碱性条件下合成了新型介孔分子筛MCM-48。研究了沸石前驱体和三乙醇胺对产物MCM-48形成的影响,XRD和TEM表征结果表明,样品具有较高的结晶度和规则的孔径;FTIR和N2吸附表征结果表明,产物MCM-48的孔壁中含有沸石的次级结构单元,从而使得样品具有更大的比表面积。产物的重芳烃轻质化反应催化活性表明,实验样品对重芳烃的转化率比常规的MCM-48高,转化率约高出11%,进一步证明了实验样品的孔壁中含有沸石的结构单元。

【Abstract】 Mesoporous aluminosilicate MCM-48 containing zeolite secondary building units in the pore wall,has been synthesized in alkaline media by a two-step procedure: the zeolite structure precursor was first synthesized by carefully controlling reaction conditions and then the pre-synthesized zeolite precursor was assembled using mixed templates of gemini surfactant [C18H37N(CH32(CH23N(CH32 C18H37]2+ and triethanolamine(TEA).Small angle XRD patterns of the as-made samples display strong diffraction peaks,indicating the highly ordered mesostructured MCM-48 was formed.TEM images further show that the as-made sample has uniform cubic pore channel system with the pore diameter of about 2.5nm.FT-IR technique was employed to characterize the pore wall of the MCM-48 containing zeolite building units.IR spectra reveal an extra band at 520cm-1600cm-1 assigned to five-membered rings from zeolite structure,suggesting the presence of zeolite building units in the pore wall.N2 adsorption/desorption result shows the material has much higher specific surface area(1200m2/g),compared with the reported data(1100m2/g) of MCM-48.This may be ascribed to the presence of micropores produced by zeolite secondary building units in its pore wall.The hydrogenation dealkylation reaction of heavy aromatic hydrocarbons on the as-made MCM-48 catalyst gives higher conversion than that on traditional MCM-48.Thus,it is concluded that as-made MCM-48 containing the secondary building units of zeolites is of potential application in the catalytic conversion of large molecules.The key factors in our synthesis of MCM-48 are the controlled preparation of zeolite precursor and the selection of auxiliary template.

【基金】 国家自然科学基金(20476060);国家重点基础研究发展规划(973计划,2004CB719704)
  • 【文献出处】 燃料化学学报 ,Journal of Fuel Chemistry and Technology , 编辑部邮箱 ,2006年01期
  • 【分类号】O643.36
  • 【被引频次】4
  • 【下载频次】270
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