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  One-Pot Cooperation of Single-Atom Rh and Ru Solid Catalysts for a Selective Tandem Olefin Isomerization-Hydrosilylation Process

Sarma, B. B., Kim, J., Amsler, J., Agostini, G., Weidenthaler, C., Pfänder, N., et al. (2020). One-Pot Cooperation of Single-Atom Rh and Ru Solid Catalysts for a Selective Tandem Olefin Isomerization-Hydrosilylation Process. Angewandte Chemie, International Edition, 59(14), 5806-5815. doi:10.1002/anie.201915255.

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 Creators:
Sarma, Bidyut B.1, Author              
Kim, Jonglack2, Author              
Amsler, Jonas3, Author
Agostini, Giovanni4, Author
Weidenthaler, Claudia5, Author              
Pfänder, Norbert6, Author              
Arenal, Raul7, 8, 9, Author
Concepción, Patricia10, Author
Plessow, Philipp3, Author
Studt, Felix3, 11, Author
Prieto, Gonzalo2, 10, Author              
Affiliations:
1Research Department Schüth, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1445589              
2Research Group Prieto, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_2243639              
3Institute of Catalysis Research and Technology (IKFT), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz Platz 1, 76344 Eggenstein-Leopoldshafen, Germany, ou_persistent22              
4ALBA Synchrotron Light Source, Carrer de la Llum 2–26, Cerdanyola del Vallès, Barcelona, Spain, ou_persistent22              
5Research Group Weidenthaler, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1950291              
6Research Department Schlögl, Max Planck Institute for Chemical Energy Conversion, Max Planck Society, ou_3023874              
7Laboratorio de Microscopias Avanzadas (LMA), Instituto de Nanociencia de Aragon (INA), Universidad de Zaragoza, Mariano Esquillor s/n, 50018 Zaragoza, Spain, ou_persistent22              
8Instituto de Ciencias de Materiales de Aragon, CSIC-Universidad de Zaragoza, Pedro Cerbuna 12, 50009 Zaragoza, Spain, ou_persistent22              
9ARAID Foundation, 50018 Zaragoza, Spain, ou_persistent22              
10ITQ Instituto de Tecnología Química, Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas (UPV-CSIC), Av. Los Naranjos s/n, 46022 Valencia, Spain, ou_persistent22              
11Institute for Chemical Technology and Polymer Chemistry (ITCP), Karlsruhe Institute of Technology (KIT), Kaiserstrasse 12, 76131 Karlsruhe, Germany, ou_persistent22              

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Free keywords: DFT calculations; olefin valorization; single-atom-catalysis; structure-performance relationships; tandem catalysis
 Abstract: Realizing the full potential of oxide‐supported single‐atom metal catalysts (SACs) is key to successfully bridge the gap between the fields of homogeneous and heterogeneous catalysis. Here we show that the one‐pot combination of Ru1/CeO2 and Rh1/CeO2 SACs enables a highly selective olefin isomerization‐hydrosilylation tandem process, hitherto restricted to molecular catalysts in solution. Individually, monoatomic Ru and Rh sites show a remarkable reaction specificity for olefin double‐bond migration and anti‐Markovnikov α‐olefin hydrosilylation, respectively. First‐principles DFT calculations ascribe such selectivity to differences in the binding strength of the olefin substrate to the monoatomic metal centers. The single‐pot cooperation of the two SACs allows the production of terminal organosilane compounds with high regio‐selectivity (>95 %) even from industrially‐relevant complex mixtures of terminal and internal olefins, alongside a straightforward catalyst recycling and reuse. These results demonstrate the significance of oxide‐supported single‐atom metal catalysts in tandem catalytic reactions, which are central for the intensification of chemical processes.

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Language(s): eng - English
 Dates: 2019-11-292019-12-302020-01-052020-03-27
 Publication Status: Published in print
 Pages: 10
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1002/anie.201915255
 Degree: -

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Title: Angewandte Chemie, International Edition
  Abbreviation : Angew. Chem., Int. Ed.
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: - Volume / Issue: 59 (14) Sequence Number: - Start / End Page: 5806 - 5815 Identifier: ISSN: 1433-7851
CoNE: https://pure.mpg.de/cone/journals/resource/1433-7851