Aromatization of n-butane and 1-butene over supported Mo2C catalyst

F. Solymosi, Aleksandar Széchenyi

Research output: Contribution to journalArticle

38 Citations (Scopus)

Abstract

The reaction pathways of n-butane were investigated on Mo2C deposited on ZSM-5 and SiO2. Particular attention was paid to the effects of the composition of ZSM-5, to the influence of the Mo2C loading, and to the nature of supports. ZSM-5 itself catalyzed the reaction of n-butane well above 800 K. Its efficiency sensitively depended on the composition of zeolite. Whereas the conversion of butane was ∼90% on ZSM-5 with SiO2/Al2O3=30 at 823 K, this value was only ∼24% on the sample with SiO2/Al2O 3=280. The dominant reaction was the cracking of butane yielding several C1-C3 compounds. Deposition of Mo2C markedly changed the catalytic performance of ZSM-5, and the dehydrogenation and the aromatization processes came into prominence. This is particularly true in the case of less effective ZSM-5 (SiO2/Al2O 3=280). From the extrapolation of selectivities to zero conversion we obtained that methane, ethane, ethylene, propylene, butene, and hydrogen are the primary products on pure and Mo2C-containing ZSM-5. Aromatics are formed in a secondary process, in the oligomerization and aromatization of butenes. The favorable effect of Mo2C is well exhibited in the case of SiO2, which was practically inactive. For 2% Mo 2C/SiO2 at 823 K the selectivity of aromatics was 16-17% at a butane conversion of 26%. On this sample the main reaction was the dehydrogenation process. As the starting compound in the formation of aromatics is very likely butene, detailed measurements were performed on its reaction on the previously studied catalysts. 1-Butene exhibited a very high reactivity on pure ZSM-5 samples even at 723 K. The presence of 2% Mo2C on the zeolites resulted only in a slight change in the conversion and product selectivities. The possible mechanism of the reactions and the role of Mo 2C are discussed, taking into account our surface science studies on the reaction of butyl species on a Mo2C/Mo(100) surface.

Original languageEnglish
Pages (from-to)221-231
Number of pages11
JournalJournal of Catalysis
Volume223
Issue number1
DOIs
Publication statusPublished - Apr 1 2004

Fingerprint

Aromatization
Butane
butenes
butanes
Butenes
Catalyst supports
catalysts
Zeolites
Dehydrogenation
selectivity
dehydrogenation
Oligomerization
Ethane
Methane
Chemical analysis
Extrapolation
Propylene
Hydrogen
Ethylene
products

Keywords

  • Aromatization of n -butane
  • MoC/SiO
  • MoC/ZSM-5
  • Reaction of 1-butene

ASJC Scopus subject areas

  • Catalysis
  • Process Chemistry and Technology

Cite this

Aromatization of n-butane and 1-butene over supported Mo2C catalyst. / Solymosi, F.; Széchenyi, Aleksandar.

In: Journal of Catalysis, Vol. 223, No. 1, 01.04.2004, p. 221-231.

Research output: Contribution to journalArticle

Solymosi, F. ; Széchenyi, Aleksandar. / Aromatization of n-butane and 1-butene over supported Mo2C catalyst. In: Journal of Catalysis. 2004 ; Vol. 223, No. 1. pp. 221-231.
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N2 - The reaction pathways of n-butane were investigated on Mo2C deposited on ZSM-5 and SiO2. Particular attention was paid to the effects of the composition of ZSM-5, to the influence of the Mo2C loading, and to the nature of supports. ZSM-5 itself catalyzed the reaction of n-butane well above 800 K. Its efficiency sensitively depended on the composition of zeolite. Whereas the conversion of butane was ∼90% on ZSM-5 with SiO2/Al2O3=30 at 823 K, this value was only ∼24% on the sample with SiO2/Al2O 3=280. The dominant reaction was the cracking of butane yielding several C1-C3 compounds. Deposition of Mo2C markedly changed the catalytic performance of ZSM-5, and the dehydrogenation and the aromatization processes came into prominence. This is particularly true in the case of less effective ZSM-5 (SiO2/Al2O 3=280). From the extrapolation of selectivities to zero conversion we obtained that methane, ethane, ethylene, propylene, butene, and hydrogen are the primary products on pure and Mo2C-containing ZSM-5. Aromatics are formed in a secondary process, in the oligomerization and aromatization of butenes. The favorable effect of Mo2C is well exhibited in the case of SiO2, which was practically inactive. For 2% Mo 2C/SiO2 at 823 K the selectivity of aromatics was 16-17% at a butane conversion of 26%. On this sample the main reaction was the dehydrogenation process. As the starting compound in the formation of aromatics is very likely butene, detailed measurements were performed on its reaction on the previously studied catalysts. 1-Butene exhibited a very high reactivity on pure ZSM-5 samples even at 723 K. The presence of 2% Mo2C on the zeolites resulted only in a slight change in the conversion and product selectivities. The possible mechanism of the reactions and the role of Mo 2C are discussed, taking into account our surface science studies on the reaction of butyl species on a Mo2C/Mo(100) surface.

AB - The reaction pathways of n-butane were investigated on Mo2C deposited on ZSM-5 and SiO2. Particular attention was paid to the effects of the composition of ZSM-5, to the influence of the Mo2C loading, and to the nature of supports. ZSM-5 itself catalyzed the reaction of n-butane well above 800 K. Its efficiency sensitively depended on the composition of zeolite. Whereas the conversion of butane was ∼90% on ZSM-5 with SiO2/Al2O3=30 at 823 K, this value was only ∼24% on the sample with SiO2/Al2O 3=280. The dominant reaction was the cracking of butane yielding several C1-C3 compounds. Deposition of Mo2C markedly changed the catalytic performance of ZSM-5, and the dehydrogenation and the aromatization processes came into prominence. This is particularly true in the case of less effective ZSM-5 (SiO2/Al2O 3=280). From the extrapolation of selectivities to zero conversion we obtained that methane, ethane, ethylene, propylene, butene, and hydrogen are the primary products on pure and Mo2C-containing ZSM-5. Aromatics are formed in a secondary process, in the oligomerization and aromatization of butenes. The favorable effect of Mo2C is well exhibited in the case of SiO2, which was practically inactive. For 2% Mo 2C/SiO2 at 823 K the selectivity of aromatics was 16-17% at a butane conversion of 26%. On this sample the main reaction was the dehydrogenation process. As the starting compound in the formation of aromatics is very likely butene, detailed measurements were performed on its reaction on the previously studied catalysts. 1-Butene exhibited a very high reactivity on pure ZSM-5 samples even at 723 K. The presence of 2% Mo2C on the zeolites resulted only in a slight change in the conversion and product selectivities. The possible mechanism of the reactions and the role of Mo 2C are discussed, taking into account our surface science studies on the reaction of butyl species on a Mo2C/Mo(100) surface.

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