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Title: The kinetics of selective oxidation of propene on bismuth vanadium molybdenum oxide catalysts

Abstract

In this study, we report the results of a systematic investigation of the kinetics of propene oxidation to acrolein over Bi 1-$x$/3V 1-$x$Mo $x$O 4. BET isotherms were measured to determine catalyst surface area, and powder X-ray diffraction was used to characterize the bulk structure. Further characterization by X-ray absorption near-edge spectroscopy (XANES) was used to determine the oxidation states of Bi, Mo, and V before and after exposure of the catalyst to propene at 713 K. We find that, contrary to previous discussions of the mechanism of propene oxidation on Bi 1-$x$/3V 1-$x$Mo $x$O 4, Bi remains in the 3+ state and only V and Mo undergo reduction and oxidation during reaction. The kinetics of propene oxidation were examined to establish the activation barrier for acrolein formation, and how the partial pressure dependences on propene and oxygen change with the value of $x$. The data obtained from this study were then used to propose a generalized model for the kinetics of propene oxidation over Bi 1-$x$/3V 1-$x$Mo $x$O 4 that is consistent with our findings about the reducibility of the three metallic elements in the oxide. According to this model, vanadium and molybdenum are randomly distributed to form threemore » types of sites each associated with its own rate parameters. MoV sites are found to exhibit the highest activity. The proposed model provides a good description of the experimental data for all catalyst formulations examined, for a range of propene and oxygen partial pressures, and for temperatures above 653 K.« less

Authors:
 [1];  [1];  [1]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Chemical Engineering
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1570979
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Catalysis
Additional Journal Information:
Journal Volume: 308; Journal Issue: C; Journal ID: ISSN 0021-9517
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; bismuth vanadium molybdenum oxide; selective oxidation; propene; acrolein

Citation Formats

Zhai, Zheng, Getsoian, Andrew “Bean”, and Bell, Alexis T. The kinetics of selective oxidation of propene on bismuth vanadium molybdenum oxide catalysts. United States: N. p., 2013. Web. doi:10.1016/j.jcat.2013.05.008.
Zhai, Zheng, Getsoian, Andrew “Bean”, & Bell, Alexis T. The kinetics of selective oxidation of propene on bismuth vanadium molybdenum oxide catalysts. United States. doi:10.1016/j.jcat.2013.05.008.
Zhai, Zheng, Getsoian, Andrew “Bean”, and Bell, Alexis T. Fri . "The kinetics of selective oxidation of propene on bismuth vanadium molybdenum oxide catalysts". United States. doi:10.1016/j.jcat.2013.05.008. https://www.osti.gov/servlets/purl/1570979.
@article{osti_1570979,
title = {The kinetics of selective oxidation of propene on bismuth vanadium molybdenum oxide catalysts},
author = {Zhai, Zheng and Getsoian, Andrew “Bean” and Bell, Alexis T.},
abstractNote = {In this study, we report the results of a systematic investigation of the kinetics of propene oxidation to acrolein over Bi1-$x$/3V1-$x$Mo$x$O4. BET isotherms were measured to determine catalyst surface area, and powder X-ray diffraction was used to characterize the bulk structure. Further characterization by X-ray absorption near-edge spectroscopy (XANES) was used to determine the oxidation states of Bi, Mo, and V before and after exposure of the catalyst to propene at 713 K. We find that, contrary to previous discussions of the mechanism of propene oxidation on Bi1-$x$/3V1-$x$Mo$x$O4, Bi remains in the 3+ state and only V and Mo undergo reduction and oxidation during reaction. The kinetics of propene oxidation were examined to establish the activation barrier for acrolein formation, and how the partial pressure dependences on propene and oxygen change with the value of $x$. The data obtained from this study were then used to propose a generalized model for the kinetics of propene oxidation over Bi1-$x$/3V1-$x$Mo$x$O4 that is consistent with our findings about the reducibility of the three metallic elements in the oxide. According to this model, vanadium and molybdenum are randomly distributed to form three types of sites each associated with its own rate parameters. MoV sites are found to exhibit the highest activity. The proposed model provides a good description of the experimental data for all catalyst formulations examined, for a range of propene and oxygen partial pressures, and for temperatures above 653 K.},
doi = {10.1016/j.jcat.2013.05.008},
journal = {Journal of Catalysis},
number = C,
volume = 308,
place = {United States},
year = {2013},
month = {6}
}

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