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

(2017) JOURNAL OF CATALYSIS. 349. p.136-148
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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 degrees 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 Bronsted 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.
Keywords
Benzene, Methanol, Dimethyl ether, Methylation, Zeolites, Methanol-to-hydrocarbons, Diphenylmethane, Formaldehyde

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Citation

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Chicago
Martinez-Espin, Juan S, Kristof De Wispelaere, Marius Westgard Erichsen, Stian Svelle, Ton VW Janssens, Veronique Van Speybroeck, Pablo Beato, and Unni Olsbye. 2017. “Benzene Co-reaction with Methanol and Dimethyl Ether over Zeolite and Zeotype Catalysts : Evidence of Parallel Reaction Paths to Toluene and Diphenylmethane.” Journal of Catalysis 349: 136–148.
APA
Martinez-Espin, J. S., De Wispelaere, K., Erichsen, M. W., Svelle, S., Janssens, T. V., Van Speybroeck, V., Beato, P., et al. (2017). Benzene co-reaction with methanol and dimethyl ether over zeolite and zeotype catalysts : evidence of parallel reaction paths to toluene and diphenylmethane. JOURNAL OF CATALYSIS, 349, 136–148.
Vancouver
1.
Martinez-Espin JS, De Wispelaere K, Erichsen MW, Svelle S, Janssens TV, Van Speybroeck V, et al. Benzene co-reaction with methanol and dimethyl ether over zeolite and zeotype catalysts : evidence of parallel reaction paths to toluene and diphenylmethane. JOURNAL OF CATALYSIS. SAN DIEGO, USA: ACADEMIC PRESS INC ELSEVIER SCIENCE; 2017;349:136–48.
MLA
Martinez-Espin, Juan S, Kristof De Wispelaere, Marius Westgard Erichsen, et al. “Benzene Co-reaction with Methanol and Dimethyl Ether over Zeolite and Zeotype Catalysts : Evidence of Parallel Reaction Paths to Toluene and Diphenylmethane.” JOURNAL OF CATALYSIS 349 (2017): 136–148. Print.
@article{8531615,
  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 degrees 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 Bronsted 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. },
  author       = {Martinez-Espin, Juan S and De Wispelaere, Kristof and Erichsen, Marius Westgard and Svelle, Stian and Janssens, Ton VW and Van Speybroeck, Veronique and Beato, Pablo and Olsbye, Unni},
  issn         = {0021-9517},
  journal      = {JOURNAL OF CATALYSIS},
  language     = {eng},
  pages        = {136--148},
  publisher    = {ACADEMIC PRESS INC ELSEVIER SCIENCE},
  title        = {Benzene co-reaction with methanol and dimethyl ether over zeolite and zeotype catalysts : evidence of parallel reaction paths to toluene and diphenylmethane},
  url          = {http://dx.doi.org/10.1016/j.jcat.2017.03.007},
  volume       = {349},
  year         = {2017},
}

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