A Mesoporous Cobalt Aluminate Spinel Catalyst for Nonoxidative Propane Dehydrogenation

Research output: Contribution to journalArticle

11 Citations (Scopus)

Abstract

A mesoporous CoAl2O4 spinel (Co-Al) is synthesized by a one-step evaporation-induced self-assembly (EISA) method. N2 physisorption and TEM are used to demonstrate the presence of mesopores within the Co-Al material. The spinel crystal structure of Co-Al, in which Co occupies tetrahedral (Td) sites, is confirmed by using XRD and UV/Vis spectroscopy. In nonoxidative propane dehydrogenation at 550 °C, a propane conversion of approximately 8 % is observed for Co-Al with a >80 % propylene selectivity, which corresponds to a turnover frequency of 5.1 h−1 based on an estimation of the number of active Co sites by using NH3 temperature-programmed desorption. A much higher propane conversion rate and a circa 80 % propylene selectivity is observed upon reaction at 600 °C. Continuous deactivation of the catalyst is observed for Co-Al at this elevated temperature. In situ X-ray absorption spectroscopy results suggest that Co remains as a Td Co2+ species under the reaction conditions. The Td Co2+ sites within the Co-Al material are thus proposed to act as Lewis acidic active sites; this acidity is verified using IR spectroscopy with pyridine as a probe molecule.

Original languageEnglish (US)
Pages (from-to)3330-3337
Number of pages8
JournalChemCatChem
Volume9
Issue number17
DOIs
StatePublished - Sep 8 2017
Externally publishedYes

Fingerprint

Propane
Dehydrogenation
dehydrogenation
Cobalt
propane
spinel
cobalt
catalysts
Catalysts
Propylene
X ray absorption spectroscopy
Physisorption
Temperature programmed desorption
Ultraviolet spectroscopy
Acidity
Pyridine
Self assembly
propylene
Infrared spectroscopy
Evaporation

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Inorganic Chemistry
  • Physical and Theoretical Chemistry
  • Organic Chemistry

Keywords

  • cobalt
  • dehydrogenation
  • mesoporous materials
  • self-assembly
  • spinel phases

Cite this

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title = "A Mesoporous Cobalt Aluminate Spinel Catalyst for Nonoxidative Propane Dehydrogenation",
abstract = "A mesoporous CoAl2O4 spinel (Co-Al) is synthesized by a one-step evaporation-induced self-assembly (EISA) method. N2 physisorption and TEM are used to demonstrate the presence of mesopores within the Co-Al material. The spinel crystal structure of Co-Al, in which Co occupies tetrahedral (Td) sites, is confirmed by using XRD and UV/Vis spectroscopy. In nonoxidative propane dehydrogenation at 550 °C, a propane conversion of approximately 8 {\%} is observed for Co-Al with a >80 {\%} propylene selectivity, which corresponds to a turnover frequency of 5.1 h−1 based on an estimation of the number of active Co sites by using NH3 temperature-programmed desorption. A much higher propane conversion rate and a circa 80 {\%} propylene selectivity is observed upon reaction at 600 °C. Continuous deactivation of the catalyst is observed for Co-Al at this elevated temperature. In situ X-ray absorption spectroscopy results suggest that Co remains as a Td Co2+ species under the reaction conditions. The Td Co2+ sites within the Co-Al material are thus proposed to act as Lewis acidic active sites; this acidity is verified using IR spectroscopy with pyridine as a probe molecule.",
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A Mesoporous Cobalt Aluminate Spinel Catalyst for Nonoxidative Propane Dehydrogenation. / Sarazen, Michele L.

In: ChemCatChem, Vol. 9, No. 17, 08.09.2017, p. 3330-3337.

Research output: Contribution to journalArticle

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AB - A mesoporous CoAl2O4 spinel (Co-Al) is synthesized by a one-step evaporation-induced self-assembly (EISA) method. N2 physisorption and TEM are used to demonstrate the presence of mesopores within the Co-Al material. The spinel crystal structure of Co-Al, in which Co occupies tetrahedral (Td) sites, is confirmed by using XRD and UV/Vis spectroscopy. In nonoxidative propane dehydrogenation at 550 °C, a propane conversion of approximately 8 % is observed for Co-Al with a >80 % propylene selectivity, which corresponds to a turnover frequency of 5.1 h−1 based on an estimation of the number of active Co sites by using NH3 temperature-programmed desorption. A much higher propane conversion rate and a circa 80 % propylene selectivity is observed upon reaction at 600 °C. Continuous deactivation of the catalyst is observed for Co-Al at this elevated temperature. In situ X-ray absorption spectroscopy results suggest that Co remains as a Td Co2+ species under the reaction conditions. The Td Co2+ sites within the Co-Al material are thus proposed to act as Lewis acidic active sites; this acidity is verified using IR spectroscopy with pyridine as a probe molecule.

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KW - spinel phases

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