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

Sarma, Bidyut B.; Kim, Jonglack; Amsler, Jonas; Agostini, Giovanni; Weidenthaler, Claudia; Pfänder, Norbert; Arenal, Raul; Concepción, Patricia; Plessow, Philipp; Studt, Felix; Prieto, Gonzalo

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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Verlagsausgabe §
DOI: 10.5445/IR/1000105846
Veröffentlicht am 06.04.2020
Originalveröffentlichung
DOI: 10.1002/anie.201915255
Scopus
Zitationen: 3
Web of Science
Zitationen: 2
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Katalyseforschung und -Technologie (IKFT)
Publikationstyp Zeitschriftenaufsatz
Publikationsjahr 2020
Sprache Englisch
Identifikator ISSN: 1433-7851
KITopen-ID: 1000105846
Erschienen in Angewandte Chemie / International edition
Band 59
Heft 14
Seiten 5806-5815
Vorab online veröffentlicht am 04.02.2020
Nachgewiesen in Scopus
Web of Science
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