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  Selective 2-Propanol Oxidation over Unsupported Co3O4 Spinel Nanoparticles: Mechanistic Insights into Aerobic Oxidation of Alcohols

Anke, S., Bendt, G., Sinev, I., Hajiyani, H. R., Antoni, H., Zegkinoglou, I., et al. (2019). Selective 2-Propanol Oxidation over Unsupported Co3O4 Spinel Nanoparticles: Mechanistic Insights into Aerobic Oxidation of Alcohols. ACS Catalysis, 9(7), 5974-5985. doi:10.1021/acscatal.9b01048.

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 Urheber:
Anke, Sven1, Autor
Bendt, Georg2, Autor
Sinev, Ilya3, Autor
Hajiyani, Hamidreza R.4, Autor
Antoni, Hendrik1, Autor
Zegkinoglou, Ioannis3, Autor
Jeon, Hyosang5, Autor           
Pentcheva, Rossitza4, Autor
Roldan Cuenya, Beatriz5, Autor           
Schulz, Stephan2, Autor
Muhler, Martin1, Autor
Affiliations:
1Laboratory of Industrial Chemistry, Ruhr Universität Bochum, ou_persistent22              
2Faculty of Chemistry, Inorganic Chemistry, and Center for Nanointegration Duisburg-Essen (CENIDE), University of Duisburg-Essen, 45114 Essen, Germany, ou_persistent22              
3Department of Physics, Ruhr-University Bochum, 44780 Bochum, Germany, ou_persistent22              
4Fakultät für Physik, Universität Duisburg-Essen, Duisburg, Germany, ou_persistent22              
5Interface Science, Fritz Haber Institute, Max Planck Society, ou_2461712              

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 Zusammenfassung: Crystalline Co3O4 nanoparticles with a uniform size of 9 nm as shown by X-ray diffraction (XRD) and transmission electron microscopy (TEM) were synthesized by thermal decomposition of cobalt acetylacetonate in oleyl amine and applied in the oxidation of 2-propanol after calcination. The catalytic properties were derived under continuous flow conditions as function of temperature up to 573 K in a fixed-bed reactor at atmospheric pressure. Temperature-programmed oxidation, desorption (TPD), surface reaction (TPSR) and 2-propanol decomposition experiments were performed to study the interaction of 2-propanol and O2 with the exposed spinel surfaces. Co3O4 selectively catalyzes the oxidative dehydrogenation of 2-propanol yielding acetone and H2O and only to a minor extent the total oxidation to CO2 and H2O at higher temperatures. The superior activity of Co3O4 reaching nearly full conversion with 100% selectivity to acetone at 440 K is attributed to the high amount of active Co3+ species at the catalyst surface as well as surface-bound reactive oxygen species observed in the O2 TPD, 2-propanol TPD, TPSR, and 2-propanol decomposition experiments. Density functional theory calculations with a Hubbard U term support the identification of fivefold coordinated octahedral surface Co5c3+ as the active site, and oxidative dehydrogenation involving adsorbed atomic oxygen was found to be the energetically most favored pathway. The consumption of surface oxygen and reduction of Co3+ to Co2+ during 2-propanol oxidation derived from X-ray absorption spectroscopy and X-ray photoelectron spectroscopy measurements before and after reaction as well as poisoning by strongly bound carbonaceous species result in the loss of the low-temperature activity, while the high-temperature reaction pathway remained unaffected.

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Sprache(n): eng - English
 Datum: 2019-03-122019-05-23
 Publikationsstatus: Online veröffentlicht
 Seiten: 12
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1021/acscatal.9b01048
 Art des Abschluß: -

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Projektname : OPERANDOCAT - In situ and Operando Nanocatalysis: Size, Shape and Chemical State Effects
Grant ID : 725915
Förderprogramm : Horizon 2020 (H2020)
Förderorganisation : European Commission (EC)

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Titel: ACS Catalysis
  Kurztitel : ACS Catal.
Genre der Quelle: Zeitschrift
 Urheber:
Affiliations:
Ort, Verlag, Ausgabe: Washington, DC : ACS
Seiten: 12 Band / Heft: 9 (7) Artikelnummer: - Start- / Endseite: 5974 - 5985 Identifikator: ISSN: 2155-5435
CoNE: https://pure.mpg.de/cone/journals/resource/2155-5435