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  Atomic‐Scale Observation of the Metal‐Promoter Interaction in Rh‐Based Syngas Upgrading Catalysts

Huang, X., Teschner, D., Dimitrakopoulou, M., Fedorov, A., Frank, B., Kraehnert, R., et al. (2019). Atomic‐Scale Observation of the Metal‐Promoter Interaction in Rh‐Based Syngas Upgrading Catalysts. Angewandte Chemie International Edition, 58(26), 8709-87713. doi:10.1002/anie.201902750.

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 Creators:
Huang, Xing1, 2, Author              
Teschner, Detre1, 2, Author              
Dimitrakopoulou, Maria1, Author              
Fedorov, Alexey3, Author
Frank, Benjamin4, Author
Kraehnert, Ralph4, Author
Rosowski, Frank4, 5, Author
Kaiser, Harry6, Author
Schunk, Stephan6, Author
Kuretschka, Christiane5, Author
Schlögl, Robert1, 2, Author              
Willinger, Marc Georg1, 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              
3Department of Mechanical and Process Engineering, ETH Zürich, Leonhardstrasse 21, 8092 Zürich, Switzerland, ou_persistent22              
4BasCat - UniCat BASF Joint Lab, Hardenbergstraße 36, 10623 Berlin, Germany, ou_persistent22              
5BASF SE, Process Research and Chemical Engineering, Heterogeneous Catalysis, Carl-Bosch-Straße 38, 67056, Ludwigshafen, Germany, ou_persistent22              
6hte GmbH, Kurpfalzring 104, 69123 Heidelberg, Germany, ou_persistent22              

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 Abstract: The direct conversion of syngas to ethanol is a cornerstone reaction in evolving technologies of CO2 utilization and hydrogen storage, which is typically performed using promoted Rh catalysts. A rational catalyst development requires a detailed structural understanding of the activated catalyst and in particular, the specific roles that promoters play in driving the chemoselectivity of this process. Herein, we report for the first time a comprehensive and comparative atomic‐scale study of metal‐promoter interaction in silica‐supported Rh, Rh‐Mn and Rh‐Mn‐Fe catalysts by aberration‐corrected transmission electron microscopy (AC‐TEM). We uncover that while the catalytic reaction leads to the formation of a Rh carbide phase in the Rh‐Mn/SiO2 catalyst, the addition of Fe results in the formation of bimetallic Rh‐Fe alloys. The latter further improves the selectivity and prevents the carbide formation. In all promoted catalysts, the Mn is present as oxide decorating the metal particles. Based on the atomic insight presented in this work, structural and electronic modifications induced by promoters are revealed and a basis for refined theoretical models is provided.

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Language(s): eng - English
 Dates: 2019-05-072019-03-042019-05-082019-05-082019-06-24
 Publication Status: Published in print
 Pages: 5
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1002/anie.201902750
 Degree: -

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Title: Angewandte Chemie International Edition
  Other : Angew. Chem. Int. Ed.
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: 5 Volume / Issue: 58 (26) Sequence Number: - Start / End Page: 8709 - 87713 Identifier: ISSN: 1433-7851
CoNE: https://pure.mpg.de/cone/journals/resource/1433-7851