Small ZSM-5 crystals with low defect density as an effective catalyst for conversion of methanol to hydrocarbons

Document identifier: oai:DiVA.org:ltu-76102
Access full text here:10.1016/j.cattod.2019.09.023
Keyword: Engineering and Technology, Chemical Engineering, Chemical Process Engineering, Teknik och teknologier, Kemiteknik, Kemiska processer, ZSM-5, Defects, Hydrocarbons, Deactivation, MTH, IR spectroscopy, OH groups, Chemical Technology, Kemisk teknologi
Publication year: 2020
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Abstract:

This work presents the synthesis of nearly defect-free ZSM-5 nanosized crystals, prepared in fluoride medium by seeding with silicalite-1. This material was carefully characterized and its catalytic performances in the methanol to hydrocarbons (MTH) reaction were assessed. Such fluoride-based material was compared to a reference ZSM-5, produced through a conventional alkaline synthesis but from the same seeding. Despite both the materials show closely identical morphology and they have a comparable acid site population, the catalyst prepared using the fluoride route showed significantly longer lifetime in MTH compared to the catalyst prepared using conventional synthesis at high pH. The slower deactivation for the samples prepared using the fluoride route was ascribed, thanks to a thorough in situ IR spectroscopy study, to its lower density of internal defects. According to the UV-Raman characterization of coke on the spent catalyst, the fluoride-based ZSM-5 catalyst produces less molecular coke species, most probably because of the absence of enlarged cavities/channels as due to the presence of internal defects. On the basis of these observations, the deactivation mechanism in the ZSM-5 synthesized by fluoride medium could be mostly related to the deposition of an external layer of bulk coke, whereas in the alkali-synthesized catalyst an additional effect from molecular coke accumulating within the porous network accelerates the deactivation process.

Authors

Mattias Grahn

Luleå tekniska universitet; Kemiteknik
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Abrar Faisal

Luleå tekniska universitet; Kemiteknik; Department of Chemical Engineering, COMSATS University Islamabad, Lahore Campus, Lahore, Pakistan
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Olov G.W Öhrman

Luleå tekniska universitet; Kemiteknik; RISE ETC - Energy Technology Center, SE-941 28 Piteå, Sweden
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Ming Zhou

Luleå tekniska universitet; Kemiteknik
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Matteo Signorile

Department of Chemistry, NIS and INSTM Reference Centre, Università di Torino, Torino, Italy
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Valentina Crocellà

Department of Chemistry, NIS and INSTM Reference Centre, Università di Torino, Torino, Italy
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Mohammad Sadegh Nabavi

Luleå tekniska universitet; Kemiteknik
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Jonas Hedlund

Luleå tekniska universitet; Kemiteknik
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