M. Westgård Erichsen

Benzene co-reaction with methanol and dimethyl ether over zeolite and zeotype catalysts: Evidence of parallel reaction paths to toluene and diphenylmethane

J. S. Martínez-Espín, K. De Wispelaere, M. Westgård Erichsen, S. Svelle, T. V. Janssens, V. Van Speybroeck, P. Beato, U. Olsbye
Journal of Catalysis
349, 136-148
2017
A1

Abstract 

The reactivity of methanol (MeOH) and dimethyl ether (DME) toward benzene was studied over zeolitic materials with different topology and acid strength (H-ZSM-5, H-SSZ-24, and H-SAPO-5) at 250–350 °C. Higher rates of methylation, and subsequent de-alkylation reactions, were observed with DME compared to MeOH. In addition, significant differences in product distribution based on the choice of methylating agent were observed. For reactions between MeOH and benzene a fraction of diphenylmethanes (DPMs) was formed, while this product group was nearly absent during reactions between DME and benzene. A range of co-feed and isotopic labeling experiments was performed, mainly over H-ZSM-5, in order to elucidate mechanistic information on the pathway from methanol and benzene to DPMs. Overall, these studies revealed that DPM formation involves the dehydrogenation of methanol to formaldehyde on the Brønsted acid site, followed by subsequent reaction with two benzene molecules. Theoretical calculations confirmed the higher reactivity of DME compared to MeOH toward benzene methylation and suggested a plausible route from formaldehyde and benzene to DPM.

Open Access version available at UGent repository
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The effects of methanol or dimethyl ether as methylating agent during zeolite catalysed benzene methylation

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Conference / event / venue 

12th European Congress on Catalysis (Europacat XII)
Kazan, Russia
Sunday, 30 August, 2015 to Friday, 4 September, 2015

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ZMPC2015
Sapporo, Japan
Sunday, 28 June, 2015 to Thursday, 2 July, 2015

Combined theoretical and experimental study on the influence of catalyst acid strength on the zeolite-catalyzed methanol conversion process

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Gent, Belgium
Tuesday, 7 October, 2014

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16th Nordic Symposium on Catalysis (NSC2014)
Oslo, Norway
Sunday, 15 June, 2014 to Tuesday, 17 June, 2014

Dynamic ab initio study towards new hydrocarbon pool cycles for the MTO-conversion in H-SAPO-5

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XVth Netherlands' Catalysis and Chemistry Conference (NCCC XV)
Noordwijkerhout, The Netherlands
Monday, 10 March, 2014 to Wednesday, 12 March, 2014
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