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Reversible Transformation of Pt Nanoparticles into Single Atoms inside High-Silica Chabazite Zeolite

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Reversible Transformation of Pt Nanoparticles into Single Atoms inside High-Silica Chabazite Zeolite

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dc.contributor.author Moliner Marin, Manuel es_ES
dc.contributor.author Gabay, Jadeene E. es_ES
dc.contributor.author Kliewer, Chris E. es_ES
dc.contributor.author Carr, Robert T. es_ES
dc.contributor.author Guzman, Javier es_ES
dc.contributor.author Casty, Gary L. es_ES
dc.contributor.author Serna Merino, Pedro Manuel es_ES
dc.contributor.author Corma Canós, Avelino es_ES
dc.date.accessioned 2017-05-22T08:30:32Z
dc.date.issued 2016-12-07
dc.identifier.issn 0002-7863
dc.identifier.uri http://hdl.handle.net/10251/81554
dc.description.abstract [EN] We report the encapsulation of platinum species in highly siliceous chabazite (CHA) crystallized in the presence of N,N,N-trimethyl-1-adamantammonium and a thiol-stabilized Pt complex. When compared to Pt/SiO2 or Pt-containing Al-rich zeolites, the materials in this work show enhanced stability toward metal sintering in a variety of industrial conditions, including H-2, O-2, and H2O. Remarkably, temperatures in the range 650-750 degrees C can be reached without significant sintering of the noble metal. Detailed structural determinations by X-ray absorption spectroscopy and aberration-corrected high-angle annular dark-field scanning transmission electron microscopy demonstrate subtle control of the supported metal structures from similar to 1 nm nanoparticles to site-isolated single Pt atoms via reversible interconversion of one species into another in reducing and oxidizing atmospheres. The combined used of microscopy and spectroscopy is critical to understand these surface-mediated transformations. When tested in hydrogenation reactions, Pt/CHA converts ethylene (similar to 80%) but not propylene under identical conditions, in contrast to Pt/SiO2, which converts both at similar rates. These differences are attributed to the negligible diffusivity of propylene through the small-pore zeolite and provide final evidence of the metal encapsulation. es_ES
dc.description.sponsorship This work has been supported by the European Union through the SYNCATMATCH project (Grant Agreement No. 671093) and the Spanish Government through "Severo Ochoa Program" (SEV 2012-0267) and MAT2015-71261-R. This research used beamline 9-BM of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. The Electron Microscopy Service of the UPV is acknowledged for their help in sample characterization. We thank Isabel Millet and Paul Stevens for technical assistance, and Randall Meyer, Aaron Sattler, and Dave Marler for review of the manuscript. We appreciate the support of ExxonMobil Research and Engineering for our efforts in fundamental catalytic research. en_EN
dc.language Inglés es_ES
dc.publisher American Chemical Society es_ES
dc.relation.ispartof Journal of the American Chemical Society es_ES
dc.rights Reserva de todos los derechos es_ES
dc.subject Small-pore zeolites es_ES
dc.subject Metal-clusters es_ES
dc.subject Hydrogen spillover es_ES
dc.subject Catalytic-properties es_ES
dc.subject Consequences es_ES
dc.subject Precursors es_ES
dc.subject Reactivity es_ES
dc.subject Encapsulation es_ES
dc.subject Performance es_ES
dc.subject Selectivity es_ES
dc.subject Electron Microscopy Service of the UPV
dc.subject.classification QUIMICA ORGANICA es_ES
dc.title Reversible Transformation of Pt Nanoparticles into Single Atoms inside High-Silica Chabazite Zeolite es_ES
dc.type Artículo es_ES
dc.embargo.lift 10000-01-01
dc.embargo.terms forever es_ES
dc.identifier.doi 10.1021/jacs.6b10169
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/MINECO//MAT2015-71261-R/ES/DISEÑO RACIONAL DE MATERIALES ZEOLITICOS CON CENTROS METALICOS PARA SU APLICACION EN PROCESOS QUIMICOS SOSTENIBLES, MEDIOAMBIENTALES Y ENERGIAS RENOVABLES/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/MINECO//SEV-2012-0267/ES/SEV-2012-0267/
dc.relation.projectID info:eu-repo/grantAgreement/DOE//DE-AC02-06CH11357/
dc.rights.accessRights Abierto es_ES
dc.contributor.affiliation Universitat Politècnica de València. Escuela Técnica Superior de Ingenieros Industriales - Escola Tècnica Superior d'Enginyers Industrials 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 Moliner Marin, M.; Gabay, JE.; Kliewer, CE.; Carr, RT.; Guzman, J.; Casty, GL.; Serna Merino, PM.... (2016). Reversible Transformation of Pt Nanoparticles into Single Atoms inside High-Silica Chabazite Zeolite. Journal of the American Chemical Society. 138(48):15743-15750. https://doi.org/10.1021/jacs.6b10169 es_ES
dc.description.accrualMethod S es_ES
dc.relation.publisherversion http://doi.org/10.1021/jacs.6b10169 es_ES
dc.description.upvformatpinicio 15743 es_ES
dc.description.upvformatpfin 15750 es_ES
dc.type.version info:eu-repo/semantics/publishedVersion es_ES
dc.description.volume 138 es_ES
dc.description.issue 48 es_ES
dc.relation.senia 328468 es_ES
dc.identifier.pmid 27934002
dc.contributor.funder European Commission
dc.contributor.funder Ministerio de Ciencia e Innovación
dc.contributor.funder U.S. Department of Energy
dc.contributor.funder Argonne National Laboratory


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