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

Zhai, Zheng; Getsoian, Andrew “Bean”; Bell, Alexis T.

doi:10.1016/j.jcat.2013.05.008

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

Journal Article · Fri Jun 14 00:00:00 EDT 2013 · Journal of Catalysis

DOI:https://doi.org/10.1016/j.jcat.2013.05.008· OSTI ID:1570979

Zhai, Zheng ^[1]; Getsoian, Andrew “Bean” ^[1]; Bell, Alexis T. ^[1]

Univ. of California, Berkeley, CA (United States). Dept. of Chemical Engineering

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_$$x$$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 Bi_1-$$x$$/3V_1-$$x$$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 Bi_1-$$x$$/3V_1-$$x$$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.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1570979

Alternate ID(s):: OSTI ID: 1110432

Journal Information:: Journal of Catalysis, Journal Name: Journal of Catalysis Journal Issue: C Vol. 308; ISSN 0021-9517

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
acrolein
bismuth vanadium molybdenum oxide
propene
selective oxidation

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

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