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分级MFI沸石与氧化铝在烯烃交叉复分解反应中的协同作用与组成的关系。

Synergism between hierarchical MFI zeolites and alumina in alkene cross-metathesis reactions as a function of composition.

作者信息

Wei Ning, Zhang Weiping, Zhang Dazhi, Huang Shengjun

机构信息

Division of Fossil Energy Conversion, Dalian Institute of Chemical Physics, Chinese Academy of Sciences Dalian 116023 China

University of Chinese Academy of Sciences Beijing 100049 China.

出版信息

RSC Adv. 2023 Apr 24;13(19):12670-12676. doi: 10.1039/d3ra01642k.

Abstract

Synergism between hierarchical zeolites and alumina in the preparation of active Mo catalysts, as a function of composition ratios, has been demonstrated in the cross-metathesis reaction between ethene and 2-butene. The metathesis reaction activity, reflected by ethene conversion, increases from 24.1% to 49.2% with the increase in the alumina content in composites from 10 wt% to 30 wt%. A further increase in the alumina content leads to the reduction in the metathesis activity, in which the ethene conversion decreases from 30.3% to 4.8% upon the enhanced alumina content from 50 wt% to 90 wt%. The impact of alumina content on the metathesis activity is closely associated with the interaction mode between the hierarchical ZSM-5 zeolite and alumina. TEM observation as well as EDS analysis and XPS results prove the progressive coating of alumina phase on the surface of zeolites along with the progressive enhancement of alumina content. The moderate alumina content in the composite enables the desired interaction between hierarchical zeolites and alumina, which is beneficial for the preparation of active catalysts for the alkene cross-metathesis reaction.

摘要

在乙烯与2-丁烯的交叉复分解反应中,已证明分级沸石与氧化铝在制备活性钼催化剂时,作为组成比的函数存在协同作用。以乙烯转化率反映的复分解反应活性,随着复合材料中氧化铝含量从10 wt%增加到30 wt%,从24.1%提高到49.2%。氧化铝含量进一步增加导致复分解活性降低,其中随着氧化铝含量从50 wt%提高到90 wt%,乙烯转化率从30.3%降至4.8%。氧化铝含量对复分解活性的影响与分级ZSM-5沸石和氧化铝之间的相互作用模式密切相关。TEM观察以及EDS分析和XPS结果证明,随着氧化铝含量的逐步增加,氧化铝相在沸石表面逐渐包覆。复合材料中适度的氧化铝含量使得分级沸石与氧化铝之间能够产生所需的相互作用,这有利于制备用于烯烃交叉复分解反应的活性催化剂。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/3d0d/10123496/0ded49ccb310/d3ra01642k-s1.jpg

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