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

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

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dc.contributor.author Sarma, Bidyut B. es_ES
dc.contributor.author Kim, Jonglack es_ES
dc.contributor.author Amsler, Jonas es_ES
dc.contributor.author Agostini, Giovanni es_ES
dc.contributor.author Weidenthaler, Claudia es_ES
dc.contributor.author Pfaender, Norbert es_ES
dc.contributor.author Arenal, Raul es_ES
dc.contributor.author Concepción Heydorn, Patricia es_ES
dc.contributor.author Plessow, Philipp es_ES
dc.contributor.author Studt, Felix es_ES
dc.contributor.author Prieto González, Gonzalo es_ES
dc.date.accessioned 2021-04-17T03:32:25Z
dc.date.available 2021-04-17T03:32:25Z
dc.date.issued 2020-03-27 es_ES
dc.identifier.issn 1433-7851 es_ES
dc.identifier.uri http://hdl.handle.net/10251/165277
dc.description.abstract [EN] 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 Ru-1/CeO2 and Rh-1/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 alpha-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. es_ES
dc.description.sponsorship X-ray absorption experiments were performed at the ALBA Synchrotron Light Source (Spain), experiments 2018082961 and 2019023278. L. Simonelli and C. Marini (CLAESSALBA beamline) are thanked for beamline setup. E. Andres, M. E. Martinez, M. Garcia, and I. Lopez (ITQ), are acknowledged for their assistance with XAS experiments. J. Buscher, J. Ternedien, B. Spliethoff, and C. Wirtz (MPI-KOFO) are acknowledged for the performance of XPS, XRD, BF-TEM and 2H NMR experiments, respectively. I. C. de Freitas (MPIKOFO) is thanked for assistance with Raman spectroscopy. J. M. Salas (ITQ) is gratefully acknowledged for his contribution to CO-FTIR experiments. J. J. Barnes and Shell (Amsterdam) are acknowledged for kindly providing an industrial olefin mixture as feed. Authors are thankful to F. Schuth for the provision of lab space and continued support. Part of the HRSTEM and EDX-STEM studies were conducted at the Laboratorio de Microscopias Avanzadas, Instituto de Nanociencia de Aragon, Universidad de Zaragoza, Spain. R.A. gratefully acknowledges the support from the Spanish Ministry of Economy and Competitiveness (MINECO) through project grant MAT2016-79776-P (AEI/FEDER, UE) and from the European Union H2020 programs "ESTEEM3" (823717). The authors acknowledge support by the state of Baden-Wurttemberg through bwHPC (bwUnicluster and JUSTUS, RV bw17D01), by the GRK 2450 and by the Helmholtz Association. This research received funding from the Max Planck Society, and the Fonds der Chemische Industrie of Germany. Funding from the Spanish Ministry of Science, Innovation and Universities (Severo Ochoa program SEV-2016-0683 and grant RTI2018096399-A-I00) is also acknowledged. B.B.S. acknowledges the Alexander von Humboldt Foundation for a postdoctoral scholarship. Open Access funding is provided by the Max Planck Society. es_ES
dc.language Inglés es_ES
dc.publisher John Wiley & Sons es_ES
dc.relation.ispartof Angewandte Chemie International Edition es_ES
dc.rights Reconocimiento (by) es_ES
dc.subject DFT calculations es_ES
dc.subject Olefin valorization es_ES
dc.subject Single-atom-catalysis es_ES
dc.subject Structure-performance relationships es_ES
dc.subject Tandem catalysis es_ES
dc.title One Pot Cooperation of Single Atom Rh and Ru Solid Catalysts for a Selective Tandem Olefin Isomerization - Hydrosilylation Process es_ES
dc.type Artículo es_ES
dc.identifier.doi 10.1002/anie.201915255 es_ES
dc.relation.projectID info:eu-repo/grantAgreement/EC/H2020/823717/EU/Enabling Science and Technology through European Electron Microscopy/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/MINECO//MAT2016-79776-P/ES/AJUSTE DE LAS PROPIEDADES OPTOELECTRONICAS DE NANOESTRUCTURAS: SU (TRANS)FORMACION Y ESTUDIOS AVANVAZADOS SOBRE SU CONFIGURACION ATOMICA Y ESTUCTURAL/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/RTI2018-096399-A-I00/ES/CLUSTERES MULTIMETALICOS Y SUBNANOMETRICOS SOPORTADOS: SINTESIS, ESTRUCTURA Y DINAMISMO ATOMICO, Y EMPLEO COMO CATALIZADORES EN LA VALORIZACION DE METANO Y ALCANOS LIGEROS/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/Baden-Württemberg Landesregierung//RV bw17D01/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/DFG//GRK 2450/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/MINECO//SEV-2016-0683/ es_ES
dc.rights.accessRights Abierto es_ES
dc.contributor.affiliation Universitat Politècnica de València. Instituto Universitario Mixto de Tecnología Química - Institut Universitari Mixt de Tecnologia Química es_ES
dc.description.bibliographicCitation Sarma, BB.; Kim, J.; Amsler, J.; Agostini, G.; Weidenthaler, C.; Pfaender, N.; Arenal, R.... (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. https://doi.org/10.1002/anie.201915255 es_ES
dc.description.accrualMethod S es_ES
dc.relation.publisherversion https://doi.org/10.1002/anie.201915255 es_ES
dc.description.upvformatpinicio 5806 es_ES
dc.description.upvformatpfin 5815 es_ES
dc.type.version info:eu-repo/semantics/publishedVersion es_ES
dc.description.volume 59 es_ES
dc.description.issue 14 es_ES
dc.identifier.pmid 31903674 es_ES
dc.identifier.pmcid PMC7154713 es_ES
dc.relation.pasarela S\409684 es_ES
dc.contributor.funder Fundación Cellex es_ES
dc.contributor.funder Max Planck Society es_ES
dc.contributor.funder European Commission es_ES
dc.contributor.funder Deutsche Forschungsgemeinschaft es_ES
dc.contributor.funder Alexander von Humboldt Foundation es_ES
dc.contributor.funder Baden-Württemberg Landesregierung es_ES
dc.contributor.funder European Regional Development Fund es_ES
dc.contributor.funder Fonds der Chemischen Industrie, Alemania es_ES
dc.contributor.funder Ministerio de Economía y Competitividad es_ES
dc.contributor.funder Helmholtz Association of German Research Centers es_ES
dc.contributor.funder Agencia Estatal de Investigación es_ES
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