Non-oxidative aromatization and ethylene formation over Ga/HZSM-5 catalysts using a mixed feed of methane and ethane

Byung Jin Lee, Young Gul Hur, Do Huei Kim, Seong Ho Lee, Kwan Young Lee

Research output: Contribution to journalArticle

1 Citation (Scopus)

Abstract

The effects of the total number of acid site and gallium loading on Ga/HZSM-5 catalysts for non-oxidative aromatization and ethylene formation were investigated using a mixed feed of methane and ethane, analogous to shale gas. When the acid sites of the catalysts increased with the change in the Si/Al ratio, the total conversion of hydrocarbons and the total yield of BTX and ethylene increased, but the selectivity of ethylene tended to decrease. This suggests that the Brønsted acid sites of catalysts is responsible for the dispersion of gallium species and the aromatization of intermediate. On the other hand, when the gallium loading of HZSM-5(15)catalysts increased from 1.0 to 7.0 wt%, the ethylene yield increased, but the BTX yield decreased. The excessive gallium loading resulted in the drastic change of textural properties and the dealumination leading to the decrease of Brønsted acid sites, which caused the decrease of BTX selectivity and the increase of ethylene selectivity. In addition, with the increase of the gallium loading of the HZSM-5(15)catalysts, while the ethane conversion did not change, the methane conversion and ethylene yield gradually increased. This suggests that the dehydrogenative coupling of methane was promoted by the gallium species formed at high gallium loading catalysts such as gallyl ion. Characterizations by N 2 adsorption/desorption, ICP-AES, XRD, XPS, TEM, NH 3 -TPD, pyridine FT-IR, H 2 -TPR, AAS, and 27 Al NMR were used to investigate the relationship between the catalytic performance for aromatization and ethylene formation.

Original languageEnglish
Pages (from-to)449-459
Number of pages11
JournalFuel
Volume253
DOIs
Publication statusPublished - 2019 Oct 1

Fingerprint

Aromatization
Gallium
Ethane
Methane
Ethylene
Catalysts
Acids
Temperature programmed desorption
Hydrocarbons
ethylene
Pyridine
Desorption
X ray photoelectron spectroscopy
Nuclear magnetic resonance
Ions
Transmission electron microscopy
Adsorption

Keywords

  • BTX
  • Dehydrogenative coupling of methane
  • Ethylene
  • Ga/HZSM-5
  • Non-oxidative aromatization
  • Shale gas

ASJC Scopus subject areas

  • Chemical Engineering(all)
  • Fuel Technology
  • Energy Engineering and Power Technology
  • Organic Chemistry

Cite this

Non-oxidative aromatization and ethylene formation over Ga/HZSM-5 catalysts using a mixed feed of methane and ethane. / Lee, Byung Jin; Hur, Young Gul; Kim, Do Huei; Lee, Seong Ho; Lee, Kwan Young.

In: Fuel, Vol. 253, 01.10.2019, p. 449-459.

Research output: Contribution to journalArticle

Lee, Byung Jin ; Hur, Young Gul ; Kim, Do Huei ; Lee, Seong Ho ; Lee, Kwan Young. / Non-oxidative aromatization and ethylene formation over Ga/HZSM-5 catalysts using a mixed feed of methane and ethane. In: Fuel. 2019 ; Vol. 253. pp. 449-459.
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abstract = "The effects of the total number of acid site and gallium loading on Ga/HZSM-5 catalysts for non-oxidative aromatization and ethylene formation were investigated using a mixed feed of methane and ethane, analogous to shale gas. When the acid sites of the catalysts increased with the change in the Si/Al ratio, the total conversion of hydrocarbons and the total yield of BTX and ethylene increased, but the selectivity of ethylene tended to decrease. This suggests that the Br{\o}nsted acid sites of catalysts is responsible for the dispersion of gallium species and the aromatization of intermediate. On the other hand, when the gallium loading of HZSM-5(15)catalysts increased from 1.0 to 7.0 wt{\%}, the ethylene yield increased, but the BTX yield decreased. The excessive gallium loading resulted in the drastic change of textural properties and the dealumination leading to the decrease of Br{\o}nsted acid sites, which caused the decrease of BTX selectivity and the increase of ethylene selectivity. In addition, with the increase of the gallium loading of the HZSM-5(15)catalysts, while the ethane conversion did not change, the methane conversion and ethylene yield gradually increased. This suggests that the dehydrogenative coupling of methane was promoted by the gallium species formed at high gallium loading catalysts such as gallyl ion. Characterizations by N 2 adsorption/desorption, ICP-AES, XRD, XPS, TEM, NH 3 -TPD, pyridine FT-IR, H 2 -TPR, AAS, and 27 Al NMR were used to investigate the relationship between the catalytic performance for aromatization and ethylene formation.",
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N2 - The effects of the total number of acid site and gallium loading on Ga/HZSM-5 catalysts for non-oxidative aromatization and ethylene formation were investigated using a mixed feed of methane and ethane, analogous to shale gas. When the acid sites of the catalysts increased with the change in the Si/Al ratio, the total conversion of hydrocarbons and the total yield of BTX and ethylene increased, but the selectivity of ethylene tended to decrease. This suggests that the Brønsted acid sites of catalysts is responsible for the dispersion of gallium species and the aromatization of intermediate. On the other hand, when the gallium loading of HZSM-5(15)catalysts increased from 1.0 to 7.0 wt%, the ethylene yield increased, but the BTX yield decreased. The excessive gallium loading resulted in the drastic change of textural properties and the dealumination leading to the decrease of Brønsted acid sites, which caused the decrease of BTX selectivity and the increase of ethylene selectivity. In addition, with the increase of the gallium loading of the HZSM-5(15)catalysts, while the ethane conversion did not change, the methane conversion and ethylene yield gradually increased. This suggests that the dehydrogenative coupling of methane was promoted by the gallium species formed at high gallium loading catalysts such as gallyl ion. Characterizations by N 2 adsorption/desorption, ICP-AES, XRD, XPS, TEM, NH 3 -TPD, pyridine FT-IR, H 2 -TPR, AAS, and 27 Al NMR were used to investigate the relationship between the catalytic performance for aromatization and ethylene formation.

AB - The effects of the total number of acid site and gallium loading on Ga/HZSM-5 catalysts for non-oxidative aromatization and ethylene formation were investigated using a mixed feed of methane and ethane, analogous to shale gas. When the acid sites of the catalysts increased with the change in the Si/Al ratio, the total conversion of hydrocarbons and the total yield of BTX and ethylene increased, but the selectivity of ethylene tended to decrease. This suggests that the Brønsted acid sites of catalysts is responsible for the dispersion of gallium species and the aromatization of intermediate. On the other hand, when the gallium loading of HZSM-5(15)catalysts increased from 1.0 to 7.0 wt%, the ethylene yield increased, but the BTX yield decreased. The excessive gallium loading resulted in the drastic change of textural properties and the dealumination leading to the decrease of Brønsted acid sites, which caused the decrease of BTX selectivity and the increase of ethylene selectivity. In addition, with the increase of the gallium loading of the HZSM-5(15)catalysts, while the ethane conversion did not change, the methane conversion and ethylene yield gradually increased. This suggests that the dehydrogenative coupling of methane was promoted by the gallium species formed at high gallium loading catalysts such as gallyl ion. Characterizations by N 2 adsorption/desorption, ICP-AES, XRD, XPS, TEM, NH 3 -TPD, pyridine FT-IR, H 2 -TPR, AAS, and 27 Al NMR were used to investigate the relationship between the catalytic performance for aromatization and ethylene formation.

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