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dc.contributor.author | Garcia-Farpon, Marcos | es_ES |
dc.contributor.author | Henao-Sierra, Wilson Albeiro | es_ES |
dc.contributor.author | Plessow, Philipp N. | es_ES |
dc.contributor.author | Andres-Marcos, Eva | es_ES |
dc.contributor.author | Arenal, Raúl | es_ES |
dc.contributor.author | Marini, Carlo | es_ES |
dc.contributor.author | Agostini, Giovanni | es_ES |
dc.contributor.author | Studt, Felix | es_ES |
dc.contributor.author | Prieto González, Gonzalo | es_ES |
dc.date.accessioned | 2023-06-23T18:02:10Z | |
dc.date.available | 2023-06-23T18:02:10Z | |
dc.date.issued | 2023-01-02 | es_ES |
dc.identifier.issn | 1433-7851 | es_ES |
dc.identifier.uri | http://hdl.handle.net/10251/194519 | |
dc.description.abstract | [EN] A frontier challenge in single-atom (SA) catalysis is the design of fully inorganic sites capable of emulating the high reaction selectivity traditionally exclusive of organometallic counterparts in homogeneous catalysis. Modulating the direct coordination environment in SA sites, via the exploitation of the oxide support's surface chemistry, stands as a powerful albeit underexplored strategy. We report that isolated Rh atoms stabilized on oxygen-defective SnO2 uniquely unite excellent TOF with essentially full selectivity in the gas-phase hydroformylation of ethylene, inhibiting the thermodynamically favored olefin hydrogenation. Density Functional Theory calculations and surface characterization suggest that substantial depletion of the catalyst surface in lattice oxygen, energetically facile on SnO2, is key to unlock a high coordination pliability at the mononuclear Rh centers, leading to an exceptional performance which is on par with that of molecular catalysts in liquid media. | es_ES |
dc.description.sponsorship | This work received funding from the European Research Council (ERC-2019-CoG 864195) and project RTI2018-096399-A-I00 funded by MCIN/AEI/10.13039/501100011033/ and "ERDF A way of making Europe". M.G.F, E.A. and W.H. acknowledge support by their predoctoral grants FPU17/04701, FPU17/04751 and PRE2019-087571, respectively. R.A. acknowledges support from the Spanish MICIN (PID2019-104739GB-100/AEI/10.13039/501100011033), Government of Aragon (DGA E13-20R) and EU H2020 "ESTEEM3" (823717). P.N.P and F.S. acknowledge support by the state of Baden-Wuerttemberg through bwHPC (bwunicluster and JUSTUS, RV bw17D011) and the Helmholtz Association. XAS experiments were performed at CLAESS and NOTOS beamlines at ALBA Synchrotron with the collaboration of ALBA staff, R. Pelaez, N. Atashi and M.E. Martinez. M. Boronat is thanked for support with slab model relaxations. V. Recio, J.M. Salas, A. Munoz and M.D. Soriano are acknowledged for experimental contributions to catalyst synthesis, FTIR, Raman and XPS measurements, respectively. | 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 - No comercial - Sin obra derivada (by-nc-nd) | es_ES |
dc.subject | DFT | es_ES |
dc.subject | Olefin Valorization | es_ES |
dc.subject | Oxygen Vacancies | es_ES |
dc.subject | Single-Atom-Catalysts | es_ES |
dc.subject | X-Ray Absorption Spectroscopy | es_ES |
dc.title | Rhodium Single-Atom Catalyst Design through Oxide Support Modulation for Selective Gas-Phase Ethylene Hydroformylation | es_ES |
dc.type | Artículo | es_ES |
dc.identifier.doi | 10.1002/anie.202214048 | es_ES |
dc.relation.projectID | info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/PID2019-104739GB-I00/ES/NANOSCOPIA IN SITU EN MATERIALES DE BAJA DIMENSIONALIDAD: MODIFICACIONES ESTRUCTURALES Y QUIMICAS Y SUS EFECTOS EN LAS PROPIEDADES OPTOELECTRONICAS/ | es_ES |
dc.relation.projectID | info:eu-repo/grantAgreement/EC/H2020/864195/EU/Engineering catalyst interoperability in next-generation tandem reactions for intensified chemical processes/TANDEng | es_ES |
dc.relation.projectID | info:eu-repo/grantAgreement/EC/H2020/823717/EU/Enabling Science and Technology through European Electron Microscopy/ESTEEM3 | 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/MCIU//FPU17%2F04701/ | es_ES |
dc.relation.projectID | info:eu-repo/grantAgreement/MCIU//FPU17%2F04751/ | es_ES |
dc.relation.projectID | info:eu-repo/grantAgreement/Gobierno de Aragón//DGA E13-20R/ | es_ES |
dc.relation.projectID | info:eu-repo/grantAgreement/Baden-Württemberg Landesregierung//RV bw17D011/ | es_ES |
dc.relation.projectID | info:eu-repo/grantAgreement/MICINN//PRE2019-087571/ | es_ES |
dc.rights.accessRights | Abierto | es_ES |
dc.description.bibliographicCitation | Garcia-Farpon, M.; Henao-Sierra, WA.; Plessow, PN.; Andres-Marcos, E.; Arenal, R.; Marini, C.; Agostini, G.... (2023). Rhodium Single-Atom Catalyst Design through Oxide Support Modulation for Selective Gas-Phase Ethylene Hydroformylation. Angewandte Chemie International Edition. 62(1):1-9. https://doi.org/10.1002/anie.202214048 | es_ES |
dc.description.accrualMethod | S | es_ES |
dc.relation.publisherversion | https://doi.org/10.1002/anie.202214048 | es_ES |
dc.description.upvformatpinicio | 1 | es_ES |
dc.description.upvformatpfin | 9 | es_ES |
dc.type.version | info:eu-repo/semantics/publishedVersion | es_ES |
dc.description.volume | 62 | es_ES |
dc.description.issue | 1 | es_ES |
dc.identifier.pmid | 36315420 | es_ES |
dc.identifier.pmcid | PMC10099584 | es_ES |
dc.relation.pasarela | S\484885 | es_ES |
dc.contributor.funder | European Commission | es_ES |
dc.contributor.funder | Gobierno de Aragón | es_ES |
dc.contributor.funder | European Research Council | es_ES |
dc.contributor.funder | Agencia Estatal de Investigación | es_ES |
dc.contributor.funder | Baden-Württemberg Landesregierung | es_ES |
dc.contributor.funder | European Regional Development Fund | es_ES |
dc.contributor.funder | Ministerio de Ciencia e Innovación | es_ES |
dc.contributor.funder | Helmholtz Association of German Research Centers | es_ES |
dc.contributor.funder | Ministerio de Ciencia, Innovación y Universidades | es_ES |