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Hydrogen transfer versus methylation : on the genesis of aromatics formation in the Methanol-To-Hydrocarbons reaction over H-ZSM-5

(2017) ACS CATALYSIS. 7(9). p.5773-5780
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Abstract
The catalytic conversion of methanol (MeOH) and dimethyl ether (DME) into fuels and chemicals over zeolites (MTH process) is industrially emerging as an alternative route to conventional oil-derived processes. After 40 years of research, a detailed mechanistic understanding of the intricate reaction network is still not fully accomplished. The overall reaction is described as two competitive catalytic cycles, dominated by alkenes and arenes, which are methylated and cracked or dealkylated to form effluent products. Herein, we present the reaction of isobutene with methanol and DME as an efficient tool for measuring the relative formation rates of alkenes and arenes, and we provide detailed mechanistic insight into the hydrogen-transfer reaction. We provide experimental and theoretical evidence that manifest a strong competition of methylation and hydrogen transfer of isobutene by methanol, while methylation is substantially favored by DME. Experiments performed at higher conversion facilitate projection of the results to the product distribution obtained when using MeOH or DME as feedstock during the MTH reaction.
Keywords
zeolites, methylation, hydrogen transfer, methanol, DME, methanol-to-hydrocarbons

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Chicago
Martínez-Espín, Juan S., Kristof De Wispelaere, Ton V. W. Janssens, Stian Svelle, Karl Petter Lillerud, Pablo Beato, Veronique Van Speybroeck, and Unni Olsbye. 2017. “Hydrogen Transfer Versus Methylation : on the Genesis of Aromatics Formation in the Methanol-To-Hydrocarbons Reaction over H-ZSM-5.” Acs Catalysis 7 (9): 5773–5780.
APA
Martínez-Espín, J. S., De Wispelaere, K., Janssens, T. V. W., Svelle, S., Lillerud, K. P., Beato, P., Van Speybroeck, V., et al. (2017). Hydrogen transfer versus methylation : on the genesis of aromatics formation in the Methanol-To-Hydrocarbons reaction over H-ZSM-5. ACS CATALYSIS, 7(9), 5773–5780.
Vancouver
1.
Martínez-Espín JS, De Wispelaere K, Janssens TVW, Svelle S, Lillerud KP, Beato P, et al. Hydrogen transfer versus methylation : on the genesis of aromatics formation in the Methanol-To-Hydrocarbons reaction over H-ZSM-5. ACS CATALYSIS. American Chemical Society (ACS); 2017;7(9):5773–80.
MLA
Martínez-Espín, Juan S., Kristof De Wispelaere, Ton V. W. Janssens, et al. “Hydrogen Transfer Versus Methylation : on the Genesis of Aromatics Formation in the Methanol-To-Hydrocarbons Reaction over H-ZSM-5.” ACS CATALYSIS 7.9 (2017): 5773–5780. Print.
@article{8533997,
  abstract     = {The catalytic conversion of methanol (MeOH) and dimethyl ether (DME) into fuels and chemicals over zeolites (MTH process) is industrially emerging as an alternative route to conventional oil-derived processes. After 40 years of research, a detailed mechanistic understanding of the intricate reaction network is still not fully accomplished. The overall reaction is described as two competitive catalytic cycles, dominated by alkenes and arenes, which are methylated and cracked or dealkylated to form effluent products. Herein, we present the reaction of isobutene with methanol and DME as an efficient tool for measuring the relative formation rates of alkenes and arenes, and we provide detailed mechanistic insight into the hydrogen-transfer reaction. We provide experimental and theoretical evidence that manifest a strong competition of methylation and hydrogen transfer of isobutene by methanol, while methylation is substantially favored by DME. Experiments performed at higher conversion facilitate projection of the results to the product distribution obtained when using MeOH or DME as feedstock during the MTH reaction.},
  author       = {Mart{\'i}nez-Esp{\'i}n, Juan S. and De Wispelaere, Kristof and Janssens, Ton V. W. and Svelle, Stian and Lillerud, Karl Petter and Beato, Pablo and Van Speybroeck, Veronique and Olsbye, Unni},
  issn         = {2155-5435},
  journal      = {ACS CATALYSIS},
  keyword      = {zeolites,methylation,hydrogen transfer,methanol,DME,methanol-to-hydrocarbons},
  language     = {eng},
  number       = {9},
  pages        = {5773--5780},
  publisher    = {American Chemical Society (ACS)},
  title        = {Hydrogen transfer versus methylation : on the genesis of aromatics formation in the Methanol-To-Hydrocarbons reaction over H-ZSM-5},
  url          = {http://dx.doi.org/10.1021/acscatal.7b01643},
  volume       = {7},
  year         = {2017},
}

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