多核芳烃在含铝M41S介孔催化剂上的异丙化反应

S.B. Pu, J.B. Kim, M. Seno, T. Inui
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引用次数: 49

摘要

采用水热法制备了Al-MCM-48介孔材料(Al-MCM-48)。Al-MCM-48具有与MCM-48几乎相同的表面积、热稳定性和孔径,其酸度与Al-MCM-41相当。而在萘的异丙化反应中,Al-MCM-48表现出比Al-MCM-41更高的活性。这是由于Al-MCM-41具有较大的孔径和三维孔隙系统,比Al-MCM-41相对狭窄的一维孔隙系统更有利于分子扩散。与大孔分子筛上2,6-二异丙基萘的产率相比,A1-M41S (Al-MCM-41和Al-MCM-48)由于酸位较少,产率不高。Al-MCM-48在芘的异丙化反应中也表现出比Al-MCM-41更高的活性,并且在介孔M41S材料上的活性远高于在y型沸石上的活性。芘的异丙化反应发生在M41S的介孔内,而在y型沸石的微孔内不能产生芘衍生物。产物分布,特别是2-异丙烯/1-异丙烯在芘异丙化过程中的比例,表明M41S在规则介孔内存在形状选择性。
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Isopropylation of polynuclear aromatic hydrocarbons on Al-containing M41S mesoporous catalysts

MCM-48 with Al incorporated into the walls constructing its mesopores (Al-MCM-48) was synthesized by a hydrothermal method. Al-MCM-48 possesses almost the same surface area, thermal stability and pore size as MCM-48, and has an acidity equivalent to Al-MCM-41. However, in the isopropylation of naphthalene, Al-MCM-48 exhibits a higher activity than Al-MCM-41. This is attributed to its larger pore size and three-dimensional pore system, which is more advantageous for molecular diffusion than the relatively narrow and one-dimensional pore system of Al-MCM-41. Compared with the yields of 2,6-diisopropylnaphthalene on large-pore zeolites, those on A1-M41S (Al-MCM-41 and Al-MCM-48) are not high because of their fewer acid sites. Al-MCM-48 also shows a higher activity than Al-MCM-41 in the isopropylation of pyrene, and the activities on the mesoporous M41S materials were much higher than that on zeolite Y. Isopropylation of pyrene occurs inside the mesopores of M41S, while pyrene derivatives cannot be produced inside the micropores of zeolite Y. However, coke formation and adsorption of the reactant and/or product proceeded in the mesoporous channels and caused catalyst deactivation. The product distributions, especially the ratio of 2-isopropylpyrene/1-isopropylpyrene in pyrene isopropylation, indicate that shape selectivity occurs inside the regular mesopores of M41S.

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Author index Subject index Contents Investigation of organosilanes as structure-directing agents in zeolite synthesis The influence of gel properties on the kinetics of crystallization and particulate properties of MFI-type zeolities. I. The influence of time and temperature of gel ageing on the particulate properties of silicalite-1 microcrystals
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