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Cyclohexane Oxidative Dehydrogenation on Graphene-Oxide-Supported Cobalt Ferrite Nanohybrids: Effect of Dynamic Nature of Active Sites on Reaction Selectivity.
Kadam, Shashikant A; Sandoval, Stefania; Bastl, Zdenek; Simkovicová, Karolína; Kvítek, Libor; Jasík, Juraj; Olszówka, Joanna Elzbieta; Valtera, Stanislav; Vaidulych, Mykhailo; Morávková, Jaroslava; Sazama, Petr; Kubicka, David; Travert, Arnaud; van Bokhoven, Jeroen A; Fortunelli, Alessandro; Kleibert, Armin; Kalbác, Martin; Vajda, Stefan.
Afiliación
  • Kadam SA; Department of Nanocatalysis, J. Heyrovsky Institute of Physical Chemistry of the Czech Academy of Sciences v.v.i, Dolejskova 3, 18223 Prague, Czech Republic.
  • Sandoval S; Department of Low Dimensional Systems, J. Heyrovsky Institute of Physical Chemistry of the Czech Academy of Sciences v.v.i, Dolejskova 3, 18223 Prague, Czech Republic.
  • Bastl Z; Department of Low Dimensional Systems, J. Heyrovsky Institute of Physical Chemistry of the Czech Academy of Sciences v.v.i, Dolejskova 3, 18223 Prague, Czech Republic.
  • Simkovicová K; Department of Nanocatalysis, J. Heyrovsky Institute of Physical Chemistry of the Czech Academy of Sciences v.v.i, Dolejskova 3, 18223 Prague, Czech Republic.
  • Kvítek L; Department of Physical Chemistry, Faculty of Science, Palacký University Olomouc, 17. Listopadu 12, 77900 Olomouc, Czech Republic.
  • Jasík J; Department of Physical Chemistry, Faculty of Science, Palacký University Olomouc, 17. Listopadu 12, 77900 Olomouc, Czech Republic.
  • Olszówka JE; Department of Nanocatalysis, J. Heyrovsky Institute of Physical Chemistry of the Czech Academy of Sciences v.v.i, Dolejskova 3, 18223 Prague, Czech Republic.
  • Valtera S; Department of Nanocatalysis, J. Heyrovsky Institute of Physical Chemistry of the Czech Academy of Sciences v.v.i, Dolejskova 3, 18223 Prague, Czech Republic.
  • Vaidulych M; Department of Nanocatalysis, J. Heyrovsky Institute of Physical Chemistry of the Czech Academy of Sciences v.v.i, Dolejskova 3, 18223 Prague, Czech Republic.
  • Morávková J; Department of Mathematics, Informatics and Cybernetics, University of Chemistry and Technology Prague, Technická 5, 166 28 Prague, Czech Republic.
  • Sazama P; Department of Nanocatalysis, J. Heyrovsky Institute of Physical Chemistry of the Czech Academy of Sciences v.v.i, Dolejskova 3, 18223 Prague, Czech Republic.
  • Kubicka D; Department of Structure and Dynamics in Catalysis, J. Heyrovsky Institute of Physical Chemistry of the Czech Academy of Sciences v.v.i, Dolejskova 3, 18223 Prague, Czech Republic.
  • Travert A; Department of Structure and Dynamics in Catalysis, J. Heyrovsky Institute of Physical Chemistry of the Czech Academy of Sciences v.v.i, Dolejskova 3, 18223 Prague, Czech Republic.
  • van Bokhoven JA; Department of Petroleum Technology and Alternative Fuels, University of Chemistry and Technology Prague, Technická 5, 166 28 Prague, Czech Republic.
  • Fortunelli A; Normandie Univ., ENSICAEN, UNICAEN, CNRS, Laboratoire Catalyse et Spectrochimie, 14000 Caen, France.
  • Kleibert A; ETH Zürich, Vladimir-Prelog Weg 1, Zürich 8093, Switzerland.
  • Kalbác M; CNR-ICCOM, Consiglio Nazionale delle Ricerche, via G. Moruzzi 1, Pisa 56124, Italy.
  • Vajda S; Swiss Light Source, Paul Scherrer Institut, 5232 Villigen PSI, Switzerland.
ACS Catal ; 13(20): 13484-13505, 2023 Oct 20.
Article en En | MEDLINE | ID: mdl-37881789
In this work, we investigated cyclohexane oxidative dehydrogenation (ODH) catalyzed by cobalt ferrite nanoparticles supported on reduced graphene oxide (RGO). We aim to identify the active sites that are specifically responsible for full and partial dehydrogenation using advanced spectroscopic techniques such as X-ray photoelectron emission microscopy (XPEEM) and X-ray photoelectron spectroscopy (XPS) along with kinetic analysis. Spectroscopically, we propose that Fe3+/Td sites could exclusively produce benzene through full cyclohexane dehydrogenation, while kinetic analysis shows that oxygen-derived species (O*) are responsible for partial dehydrogenation to form cyclohexene in a single catalytic sojourn. We unravel the dynamic cooperativity between octahedral and tetrahedral sites and the unique role of the support in masking undesired active (Fe3+/Td) sites. This phenomenon was strategically used to control the abundance of these species on the catalyst surface by varying the particle size and the wt % content of the nanoparticles on the RGO support in order to control the reaction selectivity without compromising reaction rates which are otherwise extremely challenging due to the much favorable thermodynamics for complete dehydrogenation and complete combustion under oxidative conditions.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: ACS Catal Año: 2023 Tipo del documento: Article País de afiliación: República Checa Pais de publicación: Estados Unidos
Texto completo
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: ACS Catal Año: 2023 Tipo del documento: Article País de afiliación: República Checa Pais de publicación: Estados Unidos