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  Insights into structure and dynamics of (Mn,Fe)Ox-promoted Rh nanoparticles

Dimitrakopoulou, M., Huang, X., Kröhnert, J., Teschner, D., Praetz, S., Schlesiger, C., et al. (2018). Insights into structure and dynamics of (Mn,Fe)Ox-promoted Rh nanoparticles. Faraday Discussions, 208, 207-225. doi: 10.1039/C7FD00215G.

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 Creators:
Dimitrakopoulou, Maria1, Author           
Huang, Xing1, Author           
Kröhnert, Jutta1, Author           
Teschner, Detre1, 2, Author           
Praetz, Sebastian3, Author
Schlesiger, Christopher3, Author
Malzer, Wolfgang3, Author
Janke, Christiane4, Author
Schwab, Ekkehard4, Author
Rosowski, Frank4, 5, Author
Kaiser, Harry6, Author
Schunk, Stephan6, Author
Schlögl, Robert1, 2, Author           
Trunschke, Annette1, Author           
Affiliations:
1Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
2Heterogeneous Reactions, Max-Planck-Institute for Chemical Energy Conversion , Stiftstr. 34 - 36 45470 Mülheim an der Ruhr, Germany, ou_persistent13              
3Technical University of Berlin, Institute of Optics and Atomic Physics, Hardenbergstraße 36, D-10587 Berlin, Germany, ou_persistent22              
4BASF SE, Process Research and Chemical Engineering, Heterogeneous Catalysis, Carl-Bosch-Straße 38, 67056 Ludwigshafen, Germany, ou_persistent22              
5BasCat, UniCat BASF JointLab, Technische Universität Berlin, Hardenbergstraße 36, D-10587 Berlin, Germany, ou_persistent22              
6hte GmbH, Kurpfalzring 104, 69123 Heidelberg, Germany, ou_persistent22              

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 Abstract: The mutual interaction between Rh nanoparticles and manganese/iron oxide promoters in silica-supported Rh catalysts for hydrogenation of CO to higher alcohols was analyzed by applying a combination of integral techniques including temperature-programmed reduction (TPR), X-ray photoelectron spectroscopy (XPS), X-ray absorption (XAS) and Fourier transform infrared (FTIR) spectroscopy with local analysis by using high angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) in combination with energy dispersive X-ray spectroscopy (EDX). The promoted catalysts show reduced CO adsorption capacity as evidenced by FTIR spectroscopy, which is attributed to a perforated core-shell structure of the Rh nano-particles in accordance with the microstructural analysis by electron microscopy. Iron and manganese occur in low formal oxidation states between 2+ and zero in the reduced catalysts as shown by TPR and XAS. Infrared spectroscopy measured in diffuse reflectance at reaction temperature and pressure indicates that partial coverage of the Rh particles is maintained at reaction temperature under operation and that the remaining accessible metal adsorption sites might be catalytically less relevant because hydrogenation of adsorbed carbonyl species at 523 K and 30 bar hydrogen essentially failed. It is concluded that Rh0 is poisoned due to adsorption of CO under reaction conditions of CO hydrogenation. The active sites are associated either with a (Mn,Fe)Ox (x<0.25) phase or species at the interface between Rh and its co-catalyst (Mn,Fe)Ox.

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Language(s): eng - English
 Dates: 2017-12-202017-12-202018
 Publication Status: Issued
 Pages: 19
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1039/C7FD00215G
 Degree: -

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Title: Faraday Discussions
  Abbreviation : Faraday Discuss.
Source Genre: Journal
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Publ. Info: London : Royal Society of Chemistry
Pages: 19 Volume / Issue: 208 Sequence Number: - Start / End Page: 207 - 225 Identifier: ISSN: 1359-6640
CoNE: https://pure.mpg.de/cone/journals/resource/954925269326