Atomic-Scale Observation of the Metal-Promoter Interaction in Rh-Based Syngas-Upgrading Catalysts.
- Huang X Department Heterogeneous Reactions, Max Planck Institute for Chemical Energy Conversion, Stiftstrasse 34-36, 45470, Mülheim an der Ruhr, Germany.
- Teschner D Department Heterogeneous Reactions, Max Planck Institute for Chemical Energy Conversion, Stiftstrasse 34-36, 45470, Mülheim an der Ruhr, Germany.
- Dimitrakopoulou M Department of Inorganic Chemistry, Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195, Berlin, Germany.
- Fedorov A Department of Mechanical and Process Engineering, ETH Zürich, Leonhardstrasse 21, 8092, Zürich, Switzerland.
- Frank B BasCat-UniCat BASF Joint Lab, Hardenbergstraße 36, 10623, Berlin, Germany.
- Kraehnert R BasCat-UniCat BASF Joint Lab, Hardenbergstraße 36, 10623, Berlin, Germany.
- Rosowski F BasCat-UniCat BASF Joint Lab, Hardenbergstraße 36, 10623, Berlin, Germany.
- Kaiser H hte GmbH, Kurpfalzring 104, 69123, Heidelberg, Germany.
- Schunk S hte GmbH, Kurpfalzring 104, 69123, Heidelberg, Germany.
- Kuretschka C BASF SE, Process Research and Chemical Engineering, Heterogeneous Catalysis, Carl-Bosch-Straße 38, 67056, Ludwigshafen, Germany.
- Schlögl R Department Heterogeneous Reactions, Max Planck Institute for Chemical Energy Conversion, Stiftstrasse 34-36, 45470, Mülheim an der Ruhr, Germany.
- Willinger MG Department of Inorganic Chemistry, Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195, Berlin, Germany.
- Trunschke A Department of Inorganic Chemistry, Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195, Berlin, Germany.
- 2019-05-09
Published in:
- Angewandte Chemie (International ed. in English). - 2019
Rh-based catalysts
atomic-scale imaging
heterogeneous catalysis
metal-promoter interaction
syngas-to-ethanol conversion
English
The direct conversion of syngas to ethanol, typically using promoted Rh catalysts, is a cornerstone reaction in CO2 utilization and hydrogen storage technologies. A rational catalyst development requires a detailed structural understanding of the activated catalyst and the role of promoters in driving chemoselectivity. Herein, we report a comprehensive atomic-scale study of metal-promoter interactions in silica-supported Rh, Rh-Mn, and Rh-Mn-Fe catalysts by aberration-corrected (AC) TEM. 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, which further improves the selectivity and prevents the carbide formation. In all promoted catalysts, Mn is present as an oxide decorating the metal particles. Based on the atomic insight obtained, structural and electronic modifications induced by promoters are revealed and a basis for refined theoretical models is provided.
- Language
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- English
- Open access status
- green
- Identifiers
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- DOI 10.1002/anie.201902750
- PMID 31066962
- Persistent URL
- https://sonar.ch/global/documents/268680
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