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An integrated approach to the key parameters in methanol‐to‐olefins reaction catalyzed by MFI/MEL zeolite materials

Chinese Journal of Catalysis 2022年第7期43卷 1879-1893页

作者： Chuncheng Liu Evgeny A.Uslamin Sophie H.van Vreeswijk Irina Yarulina Swapna Ganapathy Bert M.Weckhuysen Freek Kapteijn Evgeny A.Pidko Inorganic Systems Engineering Department of Chemical EngineeringDelft University of TechnologyVan der Maasweg 92629 HZ Delftthe Netherlands BASF SE Process Research and Chemical EngineeringLudwigshafen 67056Germany Inorganic Chemistry and Catalysis Debye Institute for Nanomaterials ScienceUtrecht UniversityUniversiteitsweg 993854 CG Utrechtthe Netherlands Catalysis Engineering Department of Chemical EngineeringDelft University of TechnologyVan der Maasweg 92629 HZ Delftthe Netherlands

Identification of the catalyst characteristics correlating with the key performance parameters including selectivity and stability is key to the rational catalyst design. Herein we focused on the identification of property-performance relationships in the methanol-to-olefin(MTO) process by studying in detail the catalytic behaviour of MFI, MEL and their respective intergrowth zeolites. The detailed material characterization reveals that both the high production of propylene and butylenes and the large Me OH conversion capacity correlate with the enrichment of lattice al sites in the channels of the pentasil structure as identified by 27 al MAS NMR and 3-methylpentane cracking results. The lack of correlation between MTO performance and other catalyst characteristics, such as crystal size, presence of external Brønsted acid sites and al pairing suggests their less pronounced role in defining the propylene selectivity. Our analysis reveals that catalyst deactivation is rather complex and is strongly affected by the enrichment of lattice al in the intersections, the overall al-content, and crystal size. The intergrowth of MFI and MEL phases accelerates the catalyst deactivation rate.

关键词： Structure‐performance relationship Zeolite catalysis Methanol‐to‐olefin conversion al‐distribution Acidity Intergrowth MFI/MEL Pentasil

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