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  On the reversible deactivation of cobalt ferrite spinel nanoparticles applied in selective 2-propanol oxidation

Anke, S., Falk, T., Bendt, G., Sinev, I., Hävecker, M., Antoni, H., et al. (2020). On the reversible deactivation of cobalt ferrite spinel nanoparticles applied in selective 2-propanol oxidation. Journal of Catalysis, 382, 57-68. doi:10.1016/j.jcat.2019.12.007.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0005-81C7-8 Version Permalink: http://hdl.handle.net/21.11116/0000-0006-39E9-4
Genre: Journal Article

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 Creators:
Anke, Sven1, Author
Falk, Tobias1, Author
Bendt, Georg2, Author
Sinev, Ilya3, Author
Hävecker, Michael4, 5, Author              
Antoni, Hendrik1, Author
Zegkinoglou, Ioannis3, Author
Jeon, Hyosang6, Author              
Knop-Gericke, Axel4, Author              
Schlögl, Robert4, 5, Author              
Roldan Cuenya, Beatriz6, Author              
Schulz, Stephan2, Author
Muhler, Martin1, 5, Author
Affiliations:
1Laboratory of Industrial Chemistry, Ruhr-University Bochum, 44780 Bochum, Germany, ou_persistent22              
2Faculty of Chemistry, Inorganic Chemistry, and Center for Nanointegration DuisburgEssen (CENIDE), University of Duisburg-Essen, 45114 Essen, Germany, ou_persistent22              
3Department of Physics, Ruhr-University Bochum, 44780 Bochum, Germany, ou_persistent22              
4Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
5Department of Heterogeneous Reactions, Max Planck Institute for Chemical Energy Conversion, 45470 Mülheim an der Ruhr, Germany, ou_persistent22              
6Interface Science, Fritz Haber Institute, Max Planck Society, ou_2461712              

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 Abstract: CoFe2O4 nanoparticles (NPs) were synthesized by using a colloidal one-pot synthesis method based on the decomposition of metal acetylacetonates in the presence of oleyl amine. The characterization by X-ray diffraction, transmission electron microscopy and N2 physisorption revealed non-porous spinel phase CoFe2O4 NPs with an average particle size of 4 nm. The unsupported metal oxide NPs were applied in the selective oxidation of 2-propanol in a continuously operated fixed-bed reactor under quasi steady-state conditions using a heating rate of 0.5 k min-1. 2-Propanol was found to be oxidatively dehydrogenated over CoFe2O4 yielding acetone and H2O with high selectivity. Only to a minor extent dehydration to propene and total oxidation to CO2 was observed at higher temperatures. The detected low-temperature reaction pathway with maxima at 430 and 510 K was inhibited after the initial 2-propanol oxidation up to 573 K, but an oxidative treatment in O2 or N2O atmosphere led to full regeneration. No correlation between the desorbing amount or the surface oxygen species investigated by O2 temperature-programmed desorption experiments and the low-temperature activity was observed. The amounts of evolving CO2 during the TPO experiments indicate deactivation due to formation of carbonaceous species. Inhibition experiments with pre-adsorbed reaction intermediates and infrared spectroscopy identified acetate species as reversible poison, whereas carbonates are rather spectators. In addition, carbon deposition was detected by X-ray photoelectron spectroscopy, which also revealed a minor influence of cobalt reduction during the deactivation process as confirmed by X-ray absorption spectroscopy studies.

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Language(s): eng - English
 Dates: 2019-12-062019-10-172019-12-072020-02
 Publication Status: Published in print
 Pages: 12
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1016/j.jcat.2019.12.007
 Degree: -

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Project name : OPERANDOCAT - In situ and Operando Nanocatalysis: Size, Shape and Chemical State Effects
Grant ID : 725915
Funding program : Horizon 2020 (H2020)
Funding organization : European Commission (EC)

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Title: Journal of Catalysis
  Abbreviation : J. Catal.
Source Genre: Journal
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Publ. Info: Amsterdam : Elsevier
Pages: 12 Volume / Issue: 382 Sequence Number: - Start / End Page: 57 - 68 Identifier: ISSN: 0021-9517
CoNE: https://pure.mpg.de/cone/journals/resource/954922645027