Effect of chromium and boron incorporation methods on structural and catalytic properties of hierarchical ZSM-5 in the methanol-to-propylene process

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作者
Kalantari, Neda [1 ]
F. Bekheet, Maged [2 ]
Delir Kheyrollahi Nezhad, Parastoo [1 ,3 ]
O. Back, Jan [4 ]
Farzi, Ali [1 ]
Penner, Simon [3 ]
Delibaş, Nagihan [5 ]
Schwarz, Sabine [6 ]
Bernardi, Johannes [6 ]
Salari, Dariush [7 ]
Niaei, Aligholi [1 ]
机构
[1] Reactor & Catalyst Research Lab., Department of Chemical & Petroleum Engineering, University of Tabriz, Tabriz, Iran
[2] Fachgebiet Keramische Werkstoffe/Chair of Advanced Ceramic Materials, Institut für werkstoffwissenschaften und –technologien, Technische Universität Berlin, Hardenbergstr. 40, Berlin,10623, Germany
[3] Department of Physical Chemistry, University of Innsbruck, Innrain 52c, Innsbruck,A6020, Austria
[4] Management Center Innsbruck, Abteilung für Umwelt, -Verfahrens, -und Energietechnik, Universitätsstraße 15, Innsbruck,6020, Austria
[5] Department of Physics, Sakarya University, Sakarya, Turkey
[6] University Service Center for Transmission Electron Microscopy (USTEM), TU Wien, Wiedner Hauptstrasse 8-10, Vienna,A-1040, Austria
[7] Department of Applied Chemistry, Faculty of Chemistry, University of Tabriz, Tabriz, Iran
关键词
Boron incorporations - Boron-ZSM-5 - Chromium-ZSM-5 - Hierarchical - Hierarchical structures - Metal-oxide - Methanol-to-propylene process - Performance - Preferred orientations - Synthesized zeolite;
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摘要
We introduced chromium and boron into the hierarchical structure of ZSM-5 by following an incipient wet impregnation and hydrothermal synthesis approach to enhance the performance of the catalysts in the methanol-to-propylene process. Crystal structure, preferred orientation, and crystal symmetry of synthesized zeolites were discussed using Rietveld refinement and revealed that all synthesized zeolites crystallized in a monoclinic structure, whereas the boron-incorporated sample exhibited an orthorhombic symmetry. Large-scale defect-free single-crystalline structures of hierarchical zeolite created by CTAB and F127 mesoporogens are confirmed by electron microscopy and magic angle spinning nuclear magnetic resonance (MAS NMR). The formation of surface metal oxides and extra-framework metal oxides caused changes in the electronic structure of the components as visible in Si 2p and O 1s spectra. The predominant presence of OH groups and the higher Cr (VI) /Cr (III) ratio account for the better performance of impregnated chromium-ZSM-5 especially in the production of light olefins. The introduction of boron by impregnation further preserved the preferred growth orientation, hierarchical structure with high crystallinity and caused surface acidity changes in favor of increasing propylene selectivity to 67% with a propylene/ethylene ratio of close to 8. © 2022 The Korean Society of Industrial and Engineering Chemistry
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页码:168 / 182
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