Finding the active species: The conversion of methanol to aromatics over Zn-ZSM-5/alumina shaped catalysts

被引:32
|
作者
Pinilla-Herrero, Irene [1 ,2 ]
Borfecchia, Elisa [2 ,3 ,4 ]
Cordero-Lanzac, Tomas [1 ]
Mentzel, Uffe V. [2 ]
Joensen, Finn [2 ]
Lomachenko, Kirill A. [5 ]
Bordiga, Silvia [3 ,4 ]
Olsbye, Unni [1 ]
Beato, Pablo [2 ]
Svelle, Stian [1 ]
机构
[1] Univ Oslo, Dept Chem, Ctr Mat Sci & Nanotechnol SMN, N-0315 Oslo, Norway
[2] Haldor Topsoe AS Kgs, DK-2800 Lyngby, Denmark
[3] Univ Turin, Dept Chem, INSTM Reference Ctr, Via Giuria 7, I-10135 Turin, Italy
[4] Univ Turin, NIS Interdept Ctr, Via Giuria 7, I-10135 Turin, Italy
[5] European Synchrotron Radiat Facil, 71 Ave Martyrs,CS 40220, F-38043 Grenoble 9, France
关键词
Zeolite; Extrudate; Binder; XAS; X-ray absorption spectroscopy; Methanol to gasoline;
D O I
10.1016/j.jcat.2020.10.024
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The Zn-loaded zeolite ZSM-5 is an active and promising catalyst for the conversion of methanol to aromatics with high yield. In this work, we have investigated the catalytic performance of shaped Zn-ZSM-5/alumina catalysts in this reaction at industrially relevant pressures. This has been combined with extensive characterization to identify the active Zn species. It is clear that the introduction of Zn leads to an improved catalyst lifetime when the reaction is carried out at elevated pressure. A clear shift from reaction pathways leading to alkane formation to pathways leading to molecular hydrogen formation during the production of aromatics is observed. For industrial catalysts, Zn incorporation is conveniently carried out by impregnation after shaping. A significant migration of Zn into the zeolite ion exchange positions is observed upon calcination of impregnated catalysts, and it is these species that are active for the reaction. At high Zn loadings, ZnAl2O4 species observable by X-ray absorption spectroscopy, but not detectable by diffraction, are formed in the alumina binder. (C) 2020 The Authors. Published by Elsevier Inc.
引用
收藏
页码:416 / 428
页数:13
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