The Effect of Loading of Vanadia on Silica in the Oxidation of Butane

L. Owens, Harold H Kung

Research output: Contribution to journalArticle

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Abstract

The effect of vanadium loading on the structure and the catalytic behavior of silica-supported vanadium oxide catalysts in the selective oxidation of butane was investigated in a continuous flow reaction system using catalysts containing loadings of 0.53, 0.58, or 6.4 wt% vanadium supported on Davison or Cabosil silica. The lower loading samples were found to be more selective for oxidative dehydrogenation. At 520°C, with a feed of He/O2/C4H10 = 88/8/4 at a total flow rate of 100 ml/min, the total dehydrogenation selectivity on the 0.58 wt% V sample was 65 and 50% at butane conversions of 5 and 20%. respectively, whereas they were 42 and 5% on the 6.4 wt% V samples. The activation energies for the oxidation of butane were about 110 kJ/mol for the lower loading samples and 164 kJ/mol for the higher loading samples. At 520°C the activity per vanadium was comparable for the different samples. Laser Raman spectra of fresh catalysts indicated that only a well-dispersed vanadia species existed on the 0.58 wt% V sample, while crystalline V2O5 was also formed on the 6.4 wt% V samples. The ratio of well-dispersed to crystalline vanadia species on the fresh catalysts was higher for the Cabosil silica-supported sample than the Davison silica-supported sample. After reaction, the spectra of the 0.58 wt% V samples did not indicate any changes. However, significantly more crystalline V2O5 was found on the 6.4 wt% V samples on both silica supports, indicating that aggregation of vanadia had occurred during reaction. The higher total dehydrogenation selectivity on the 0.58 wt% V samples was attributed to the presence of the well-dispersed vanadia, while the presence of crystalline V2O5 species on the higher loading samples contributed to the production of total oxidation products.

Original languageEnglish
Pages (from-to)202-213
Number of pages12
JournalJournal of Catalysis
Volume144
Issue number1
DOIs
Publication statusPublished - Nov 1993

Fingerprint

Butane
butanes
Vanadium
Silicon Dioxide
Silica
silicon dioxide
Dehydrogenation
Oxidation
oxidation
Crystalline materials
Catalysts
dehydrogenation
vanadium
Oxides
catalysts
Raman scattering
Agglomeration
Activation energy
Flow rate
butane

ASJC Scopus subject areas

  • Process Chemistry and Technology
  • Catalysis

Cite this

The Effect of Loading of Vanadia on Silica in the Oxidation of Butane. / Owens, L.; Kung, Harold H.

In: Journal of Catalysis, Vol. 144, No. 1, 11.1993, p. 202-213.

Research output: Contribution to journalArticle

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abstract = "The effect of vanadium loading on the structure and the catalytic behavior of silica-supported vanadium oxide catalysts in the selective oxidation of butane was investigated in a continuous flow reaction system using catalysts containing loadings of 0.53, 0.58, or 6.4 wt{\%} vanadium supported on Davison or Cabosil silica. The lower loading samples were found to be more selective for oxidative dehydrogenation. At 520°C, with a feed of He/O2/C4H10 = 88/8/4 at a total flow rate of 100 ml/min, the total dehydrogenation selectivity on the 0.58 wt{\%} V sample was 65 and 50{\%} at butane conversions of 5 and 20{\%}. respectively, whereas they were 42 and 5{\%} on the 6.4 wt{\%} V samples. The activation energies for the oxidation of butane were about 110 kJ/mol for the lower loading samples and 164 kJ/mol for the higher loading samples. At 520°C the activity per vanadium was comparable for the different samples. Laser Raman spectra of fresh catalysts indicated that only a well-dispersed vanadia species existed on the 0.58 wt{\%} V sample, while crystalline V2O5 was also formed on the 6.4 wt{\%} V samples. The ratio of well-dispersed to crystalline vanadia species on the fresh catalysts was higher for the Cabosil silica-supported sample than the Davison silica-supported sample. After reaction, the spectra of the 0.58 wt{\%} V samples did not indicate any changes. However, significantly more crystalline V2O5 was found on the 6.4 wt{\%} V samples on both silica supports, indicating that aggregation of vanadia had occurred during reaction. The higher total dehydrogenation selectivity on the 0.58 wt{\%} V samples was attributed to the presence of the well-dispersed vanadia, while the presence of crystalline V2O5 species on the higher loading samples contributed to the production of total oxidation products.",
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