Effect of Ba addition to Ga-α-Al2O3 catalyst on structure and catalytic selectivity for dehydrogenation of ethane

Hirofumi Seki, Hikaru Saito, Kenta Toko, Yukiko Hosono, Takuma Higo, Jeong Gil Seo, Shun Maeda, Kunihide Hashimoto, Shuhei Ogo, Yasushi Sekine

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Abstract

Modified Ga-α-Al2O3 catalyst with Ba showed high catalytic activity, selectivity and low carbon formation on catalytic ethane dehydrogenation to ethylene even in the presence of steam. The resultant Ba-Ga-α-Al2O3 (Ba/Ga molar ratio = 0.10) catalyst showed high ethylene selectivity (98%), high activity, and stability. Temperature-programmed oxidation measurements revealed that Ba addition suppressed coke formation at Ga sites. XRD, XAFS and TEM results showed the existence of highly dispersed β-Ga2O3 on the α-Al2O3 support, irrespective of Ba addition. Observation of hydrogen adsorption using FT-IR spectroscopy revealed a decrease in the surface tetrahedrally coordinated Ga (designated as Ga(T)) sites by Ba modification, indicating that the surface Ga(T) sites are covered with Ba. Density functional theory calculation revealed that coke formation through ethylene decomposition is likely to occur at surface Ga(T) sites, and revealed that the addition of an optimal amount of Ba to Ga-α-Al2O3 inhibits coke formation at the surface Ga(T) sites, leading to high ethylene selectivity.

Original languageEnglish
Pages (from-to)23-30
Number of pages8
JournalApplied Catalysis A: General
Volume581
DOIs
Publication statusPublished - 2019 Jul 5

Fingerprint

Ethane
Catalyst selectivity
Dehydrogenation
Ethylene
Coke
Catalysts
Steam
Density functional theory
Hydrogen
Infrared spectroscopy
Catalyst activity
Carbon
Thermodynamic properties
Transmission electron microscopy
Decomposition
Adsorption
Oxidation
ethylene
Temperature

Keywords

  • Ba addition
  • Coke resistance
  • Ethane dehydrogenation
  • Ethylene selectivity
  • Ga catalysts

ASJC Scopus subject areas

  • Catalysis
  • Process Chemistry and Technology

Cite this

Effect of Ba addition to Ga-α-Al2O3 catalyst on structure and catalytic selectivity for dehydrogenation of ethane. / Seki, Hirofumi; Saito, Hikaru; Toko, Kenta; Hosono, Yukiko; Higo, Takuma; Gil Seo, Jeong; Maeda, Shun; Hashimoto, Kunihide; Ogo, Shuhei; Sekine, Yasushi.

In: Applied Catalysis A: General, Vol. 581, 05.07.2019, p. 23-30.

Research output: Contribution to journalArticle

Seki, Hirofumi ; Saito, Hikaru ; Toko, Kenta ; Hosono, Yukiko ; Higo, Takuma ; Gil Seo, Jeong ; Maeda, Shun ; Hashimoto, Kunihide ; Ogo, Shuhei ; Sekine, Yasushi. / Effect of Ba addition to Ga-α-Al2O3 catalyst on structure and catalytic selectivity for dehydrogenation of ethane. In: Applied Catalysis A: General. 2019 ; Vol. 581. pp. 23-30.
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T1 - Effect of Ba addition to Ga-α-Al2O3 catalyst on structure and catalytic selectivity for dehydrogenation of ethane

AU - Seki, Hirofumi

AU - Saito, Hikaru

AU - Toko, Kenta

AU - Hosono, Yukiko

AU - Higo, Takuma

AU - Gil Seo, Jeong

AU - Maeda, Shun

AU - Hashimoto, Kunihide

AU - Ogo, Shuhei

AU - Sekine, Yasushi

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N2 - Modified Ga-α-Al2O3 catalyst with Ba showed high catalytic activity, selectivity and low carbon formation on catalytic ethane dehydrogenation to ethylene even in the presence of steam. The resultant Ba-Ga-α-Al2O3 (Ba/Ga molar ratio = 0.10) catalyst showed high ethylene selectivity (98%), high activity, and stability. Temperature-programmed oxidation measurements revealed that Ba addition suppressed coke formation at Ga sites. XRD, XAFS and TEM results showed the existence of highly dispersed β-Ga2O3 on the α-Al2O3 support, irrespective of Ba addition. Observation of hydrogen adsorption using FT-IR spectroscopy revealed a decrease in the surface tetrahedrally coordinated Ga (designated as Ga(T)) sites by Ba modification, indicating that the surface Ga(T) sites are covered with Ba. Density functional theory calculation revealed that coke formation through ethylene decomposition is likely to occur at surface Ga(T) sites, and revealed that the addition of an optimal amount of Ba to Ga-α-Al2O3 inhibits coke formation at the surface Ga(T) sites, leading to high ethylene selectivity.

AB - Modified Ga-α-Al2O3 catalyst with Ba showed high catalytic activity, selectivity and low carbon formation on catalytic ethane dehydrogenation to ethylene even in the presence of steam. The resultant Ba-Ga-α-Al2O3 (Ba/Ga molar ratio = 0.10) catalyst showed high ethylene selectivity (98%), high activity, and stability. Temperature-programmed oxidation measurements revealed that Ba addition suppressed coke formation at Ga sites. XRD, XAFS and TEM results showed the existence of highly dispersed β-Ga2O3 on the α-Al2O3 support, irrespective of Ba addition. Observation of hydrogen adsorption using FT-IR spectroscopy revealed a decrease in the surface tetrahedrally coordinated Ga (designated as Ga(T)) sites by Ba modification, indicating that the surface Ga(T) sites are covered with Ba. Density functional theory calculation revealed that coke formation through ethylene decomposition is likely to occur at surface Ga(T) sites, and revealed that the addition of an optimal amount of Ba to Ga-α-Al2O3 inhibits coke formation at the surface Ga(T) sites, leading to high ethylene selectivity.

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KW - Ethylene selectivity

KW - Ga catalysts

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