A Mesoporous Cobalt Aluminate Spinel Catalyst for Nonoxidative Propane Dehydrogenation

Bo Hu, Wun Gwi Kim, Taylor P. Sulmonetti, Michele Lee Sarazen, Shuai Tan, Jungseob So, Yujun Liu, Ravindra S. Dixit, Sankar Nair, Christopher W. Jones

Research output: Contribution to journalArticle

8 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

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

Cite this

Hu, B., Kim, W. G., Sulmonetti, T. P., Sarazen, M. L., Tan, S., So, J., ... Jones, C. W. (2017). A Mesoporous Cobalt Aluminate Spinel Catalyst for Nonoxidative Propane Dehydrogenation. ChemCatChem, 9(17), 3330-3337. https://doi.org/10.1002/cctc.201700647
Hu, Bo ; Kim, Wun Gwi ; Sulmonetti, Taylor P. ; Sarazen, Michele Lee ; Tan, Shuai ; So, Jungseob ; Liu, Yujun ; Dixit, Ravindra S. ; Nair, Sankar ; Jones, Christopher W. / A Mesoporous Cobalt Aluminate Spinel Catalyst for Nonoxidative Propane Dehydrogenation. In: ChemCatChem. 2017 ; Vol. 9, No. 17. pp. 3330-3337.
@article{a765cebc897a4fd793cd5975838aa79e,
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.",
author = "Bo Hu and Kim, {Wun Gwi} and Sulmonetti, {Taylor P.} and Sarazen, {Michele Lee} and Shuai Tan and Jungseob So and Yujun Liu and Dixit, {Ravindra S.} and Sankar Nair and Jones, {Christopher W.}",
year = "2017",
month = "9",
day = "8",
doi = "https://doi.org/10.1002/cctc.201700647",
language = "English (US)",
volume = "9",
pages = "3330--3337",
journal = "ChemCatChem",
issn = "1867-3880",
publisher = "Wiley - VCH Verlag GmbH & CO. KGaA",
number = "17",

}

Hu, B, Kim, WG, Sulmonetti, TP, Sarazen, ML, Tan, S, So, J, Liu, Y, Dixit, RS, Nair, S & Jones, CW 2017, 'A Mesoporous Cobalt Aluminate Spinel Catalyst for Nonoxidative Propane Dehydrogenation', ChemCatChem, vol. 9, no. 17, pp. 3330-3337. https://doi.org/10.1002/cctc.201700647

A Mesoporous Cobalt Aluminate Spinel Catalyst for Nonoxidative Propane Dehydrogenation. / Hu, Bo; Kim, Wun Gwi; Sulmonetti, Taylor P.; Sarazen, Michele Lee; Tan, Shuai; So, Jungseob; Liu, Yujun; Dixit, Ravindra S.; Nair, Sankar; Jones, Christopher W.

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

Research output: Contribution to journalArticle

TY - JOUR

T1 - A Mesoporous Cobalt Aluminate Spinel Catalyst for Nonoxidative Propane Dehydrogenation

AU - Hu, Bo

AU - Kim, Wun Gwi

AU - Sulmonetti, Taylor P.

AU - Sarazen, Michele Lee

AU - Tan, Shuai

AU - So, Jungseob

AU - Liu, Yujun

AU - Dixit, Ravindra S.

AU - Nair, Sankar

AU - Jones, Christopher W.

PY - 2017/9/8

Y1 - 2017/9/8

N2 - 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.

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.

UR - http://www.scopus.com/inward/record.url?scp=85029000846&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85029000846&partnerID=8YFLogxK

U2 - https://doi.org/10.1002/cctc.201700647

DO - https://doi.org/10.1002/cctc.201700647

M3 - Article

VL - 9

SP - 3330

EP - 3337

JO - ChemCatChem

JF - ChemCatChem

SN - 1867-3880

IS - 17

ER -