首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Effect of Al Distribution in MFI Framework Channels on the Catalytic Performance of Ethane and Ethylene Aromatization
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Effect of Al Distribution in MFI Framework Channels on the Catalytic Performance of Ethane and Ethylene Aromatization

机译:MFI框架通道中Al分布对乙烷和乙烯芳族化催化性能的影响

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摘要

The relationship between the formation of aromatics in catalytic ethane/ethylene aromatization and Al distribution in Mobil-type five (MFI) channel was investigated using ZSM-5 zeolites with controlled Al distribution, which were obtained by employing different organic structural directing agents (OSDAs) during the ZSM-5 synthesis step. ZSM-5 samples with framework Al mainly distributed in the MFI straight/sinusoidal channels or intersections were obtained using pentaerythritol or tetrapropylammonium hydroxide as OSDAs, respectively. Samples with Al distributed in both channel and intersection were synthesized using n-butylamine as a template. Ethane aromatization results showed that Pt-modified ZSM-5 with acid sites located in the channel intersection tended to produce more aromatic compounds and less methane than that of a catalyst with acid sites located in the straight and/or sinusoidal channels under the same conversion of ethane. Ethylene aromatization was performed to understand how the intermediates evolve within acid sites. The results indicated that acid sites located in the intersection with more space void were conducive for the geometry transformation of intermediates, resulting in a much faster hydrogen transfer reaction rate than that in the straight and/or sinusoidal channels with bulky bimolecular reaction intermediates involved. Hence, ZSM-5 with acid site mainly located in the channel intersection would be more favorable for the formation of aromatics over the other two types of catalysts in ethylene aromatization.
机译:使用ZSM-5沸石采用不同的有机结构指示剂(OSDAS)来研究催化乙烷/乙烯芳香化和MOBIL型五(MFI)通道中的Al分布之间的芳烃芳烃和Al分布之间的关系。在ZSM-5合成步骤期间。使用季戊四醇或四丙基铵作为OSDAs获得主要分布在MFI直/正弦通道或交叉口中的框架Al的ZSM-5样品。使用N-丁胺作为模板,合成具有在通道和交叉处分布的Al的样品。乙烷芳族化结果表明,PT改性ZSM-5与位于通道交叉口中的酸位点倾向于产生更多的芳族化合物和甲烷,而不是位于直线和/或正弦通道中的酸位点的催化剂的催化剂埃钵。进行乙烯芳族化以了解中间体如何在酸部位内进化。结果表明,位于具有更多空间空隙的交叉点中的酸部位有利于中间体的几何形状转化,得到的氢转移反应速率比具有庞大的双分子反应中间体的直链和/或正弦通道中的较快。因此,具有主要位于通道交叉口的酸部位的ZSM-5将更有利于在乙烯芳族化中的其他两种类型的催化剂上形成芳烃。

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