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Determination of the Evolution of Heterogeneous Single Metal Atoms and Nanoclusters under Reaction Conditions: Which Are the Working Catalytic Sites?

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Determination of the Evolution of Heterogeneous Single Metal Atoms and Nanoclusters under Reaction Conditions: Which Are the Working Catalytic Sites?

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dc.contributor.author Liu, Lichen es_ES
dc.contributor.author MEIRA, DEBORA M. es_ES
dc.contributor.author Arenal, Raul es_ES
dc.contributor.author Concepción Heydorn, Patricia es_ES
dc.contributor.author Puga, Alberto V. es_ES
dc.contributor.author Corma Canós, Avelino es_ES
dc.date.accessioned 2020-09-24T12:30:20Z
dc.date.available 2020-09-24T12:30:20Z
dc.date.issued 2019-12-06 es_ES
dc.identifier.issn 2155-5435 es_ES
dc.identifier.uri http://hdl.handle.net/10251/150676
dc.description.abstract [EN] Identification of active sites in heterogeneous metal catalysts is critical for understanding the reaction mechanism at the molecular level and for designing more efficient catalysts. Because of their structural flexibility, subnanometric metal catalysts, including single atoms and clusters with a few atoms, can exhibit dynamic structural evolution when interacting with substrate molecules, making it difficult to determine the catalytically active sites. In this work, Pt catalysts containing selected types of Pt entities (from single atoms to clusters and nanoparticles) have been prepared, and their evolution has been followed, while they were reacting in a variety of heterogeneous catalytic reactions, including selective hydrogenation reactions, CO oxidation, dehydrogenation of propane, and photocatalytic H-2 evolution reaction. By in situ X-ray absorption spectroscopy, in situ IR spectroscopy, and high-resolution electron microscopy techniques, we will show that some characterization techniques carried out in an inadequate way can introduce confusion on the interpretation of coordination environment of highly dispersed Pt species. Finally, the combination of catalytic reactivity and in situ characterization techniques shows that, depending on the catalyst-reactant interaction and metal-support interaction, singly dispersed metal atoms can rapidly evolve into metal clusters or nanoparticles, being the working active sites for those abovementioned heterogeneous reactions. es_ES
dc.description.sponsorship This work has been supported by the European Union through the European Research Council (grant ERC-AdG-2014-671093, SynCatMatch) and the Spanish government through the "Severo Ochoa Program" (SEV-2016-0683). L.L. thanks ITQ for providing a contract. The authors also thank Microscopy Service of UPV for the TEM and STEM measurements. This research used resources of the Advanced Photon Source, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by Argonne National Laboratory, and was supported by the U.S. DOE under contract no. DE-AC02-06CH11357 and the Canadian Light Source and its funding partners. The HR STEM and STEM-EELS studies were conducted at the Laboratorio de Microscopias Avanzadas, Universidad de Zaragoza, Spain. R.A. acknowledges support from Spanish MINECO grant MAT2016-79776-P (AEI/FEDER, UE), from the Government of Aragon and the European Social Fund (grant number E13_17R, FEDER, UE), and from the European Union H2020 program "ESTEEM3" (grant number 823717). A.V.P. thanks the Spanish Government (Agencia Estatal de Investigacion) and the European Union (European Regional Development Fund) for a grant for young researchers (CTQ2015-74138-JIN, AEI/FEDER/UE). es_ES
dc.language Inglés es_ES
dc.publisher American Chemical Society es_ES
dc.relation DOE/DE-AC02-06CH11357 es_ES
dc.relation Agencia Estatal de Investigación/CTQ2015-74138-JIN es_ES
dc.relation MINECO/MAT2016-79776-P es_ES
dc.relation Gobierno de Aragón/E13_17R es_ES
dc.relation MINECO/SEV-2016-0683 es_ES
dc.relation.ispartof ACS Catalysis es_ES
dc.rights Reconocimiento - No comercial (by-nc) es_ES
dc.subject Single-atom catalysis es_ES
dc.subject Subnanometric clusters es_ES
dc.subject Size effect es_ES
dc.subject Platinum es_ES
dc.subject Hydrogenation of nitroarenes es_ES
dc.subject CO oxidation es_ES
dc.subject Propane dehydrogenation es_ES
dc.subject Photocatalytic H-2 evolution es_ES
dc.subject.classification QUIMICA ANALITICA es_ES
dc.subject.classification QUIMICA ORGANICA es_ES
dc.title Determination of the Evolution of Heterogeneous Single Metal Atoms and Nanoclusters under Reaction Conditions: Which Are the Working Catalytic Sites? es_ES
dc.type Artículo es_ES
dc.identifier.doi 10.1021/acscatal.9b04214 es_ES
dc.relation.projectID info:eu-repo/grantAgreement/EC/H2020/671093/EU/MATching zeolite SYNthesis with CATalytic activity/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/EC/H2020/823717/EU/Enabling Science and Technology through European Electron Microscopy/ es_ES
dc.rights.accessRights Abierto es_ES
dc.contributor.affiliation Universitat Politècnica de València. Departamento de Química - Departament de Química 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 Liu, L.; Meira, DM.; Arenal, R.; Concepción Heydorn, P.; Puga, AV.; Corma Canós, A. (2019). Determination of the Evolution of Heterogeneous Single Metal Atoms and Nanoclusters under Reaction Conditions: Which Are the Working Catalytic Sites?. ACS Catalysis. 9(12):10626-10639. https://doi.org/10.1021/acscatal.9b04214 es_ES
dc.description.accrualMethod S es_ES
dc.relation.publisherversion https://doi.org/10.1021/acscatal.9b04214 es_ES
dc.description.upvformatpinicio 10626 es_ES
dc.description.upvformatpfin 10639 es_ES
dc.type.version info:eu-repo/semantics/publishedVersion es_ES
dc.description.volume 9 es_ES
dc.description.issue 12 es_ES
dc.identifier.pmid 31840008 es_ES
dc.identifier.pmcid PMC6902617 es_ES
dc.relation.pasarela S\410560 es_ES
dc.contributor.funder Gobierno de Aragón es_ES
dc.contributor.funder Canadian Light Source es_ES
dc.contributor.funder U.S. Department of Energy es_ES
dc.contributor.funder Agencia Estatal de Investigación es_ES
dc.contributor.funder European Regional Development Fund es_ES
dc.contributor.funder Ministerio de Economía y Competitividad es_ES


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