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Exceptional oxidation activity with size-controlled supported gold clusters of low atomicity

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Exceptional oxidation activity with size-controlled supported gold clusters of low atomicity

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dc.contributor.author Corma Canós, Avelino es_ES
dc.contributor.author Concepción Heydorn, Patricia es_ES
dc.contributor.author Boronat Zaragoza, Mercedes es_ES
dc.contributor.author Sabater Picot, Mª José es_ES
dc.contributor.author Navas Escrig, Javier es_ES
dc.contributor.author Yacaman, Miguel José es_ES
dc.contributor.author Larios, Eduardo es_ES
dc.contributor.author Posadas, Álvaro es_ES
dc.contributor.author López Quintela, M. Arturo es_ES
dc.contributor.author Buceta, David es_ES
dc.contributor.author Mendoza, Ernest es_ES
dc.contributor.author Guilera, Gemma es_ES
dc.contributor.author Mayoral, Álvaro es_ES
dc.date.accessioned 2016-07-06T11:52:24Z
dc.date.available 2016-07-06T11:52:24Z
dc.date.issued 2013-09
dc.identifier.issn 1755-4330
dc.identifier.uri http://hdl.handle.net/10251/67246
dc.description.abstract [EN] The catalytic activity of gold depends on particle size, with the reactivity increasing as the particle diameter decreases. However, investigations into behaviour in the subnanometre regime (where gold exists as small clusters of a few atoms) began only recently with advances in synthesis and characterization techniques. Here we report an easy method to prepare isolated gold atoms supported on functionalized carbon nanotubes and their performance in the oxidation of thiophenol with O-2. We show that single gold atoms are not active, but they aggregate under reaction conditions into gold clusters of low atomicity that exhibit a catalytic activity comparable to that of sulfhydryl oxidase enzymes. When clusters grow into larger nanoparticles, catalyst activity drops to zero. Theoretical calculations show that gold clusters are able to activate thiophenol and O-2 simultaneously, and larger nanoparticles are passivated by strongly adsorbed thiolates. The combination of both reactants activation and facile product desorption makes gold clusters excellent catalysts. es_ES
dc.description.sponsorship Financial support from the Spanish Science and Innovation Ministry (Consolider Ingenio 2010-MULTICAT CSD2009-00050, Subprograma de apoyo a Centros y Universidades de Excelencia Severo Ochoa SEV 2012 0267, MAT2011-28009 and MAT2010-20442 projects) and Xunta de Galicia (Grupos Ref.Comp.2010/41) is acknowledged. M.J.Y. and E. L. acknowledge the support of the National Centre for Research Resources (5 G12RR013646-12) and the National Institute on Minority Health and Health Disparities (G12MD007591) from the National Institutes of Health and of the National Science Foundation for support with grants DMR-1103730 and PREM: NSF PREM Grant # DMR 0934218. We also acknowledge the support of Consejo Nacional De Ciencia y Tecnologia. J.N. expresses his gratitude to Consejo Superior de Investigaciones Cientificas for a JAE Fellowship. en_EN
dc.language Inglés es_ES
dc.publisher Nature Publishing Group es_ES
dc.relation.ispartof Nature Chemistry es_ES
dc.rights Reserva de todos los derechos es_ES
dc.subject Gold es_ES
dc.subject Gold, clusters, atomicity, oxidation, disulfides es_ES
dc.subject Clusters es_ES
dc.subject Atomicity es_ES
dc.subject Oxidation es_ES
dc.subject Disulfides es_ES
dc.subject.classification QUIMICA ORGANICA es_ES
dc.title Exceptional oxidation activity with size-controlled supported gold clusters of low atomicity es_ES
dc.type Artículo es_ES
dc.identifier.doi 10.1038/NCHEM.1721
dc.relation.projectID info:eu-repo/grantAgreement/MICINN//CSD2009-00050/ES/Desarrollo de catalizadores más eficientes para el diseño de procesos químicos sostenibles y produccion limpia de energia/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/NIH//5G12RR013646-12/US/CORE 1- BIOPHOTONICS CORE/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/NIMHD//G12MD007591/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/NSF//1103730/US/Alloys at the Nanoscale; The Case of Nanoparticles Second Phase/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/NSF//0934218/US/Oxide and Metal Nanoparticles-The Interface between Life Sciences and Physical Sciences/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/MINECO//SEV-2012-0267/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/MICINN//MAT2011-28009/ES/CATALIZADORES MONO- Y MULTIFUNCIONALES BASADOS EN NANOPARTICULAS METALICAS DIRIGIDOS A TRANSFORMACIONES SECUENCIALES O REACCIONES EN CASCADA/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/MICINN//MAT2010-20442/ES/PROPIEDADES CATALITICAS DE CLUSTERES ATOMICOS DE ELEMENTOS METALICOS/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/Xunta de Galicia//Comp.2010%2F41/ 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.contributor.affiliation Universitat Politècnica de València. Departamento de Química - Departament de Química es_ES
dc.description.bibliographicCitation Corma Canós, A.; Concepción Heydorn, P.; Boronat Zaragoza, M.; Sabater Picot, MJ.; Navas Escrig, J.; Yacaman, MJ.; Larios, E.... (2013). Exceptional oxidation activity with size-controlled supported gold clusters of low atomicity. Nature Chemistry. 5(9):775-781. https://doi.org/10.1038/NCHEM.1721 es_ES
dc.description.accrualMethod S es_ES
dc.relation.publisherversion https://dx.doi.org/10.1038/nchem.1721 es_ES
dc.description.upvformatpinicio 775 es_ES
dc.description.upvformatpfin 781 es_ES
dc.type.version info:eu-repo/semantics/publishedVersion es_ES
dc.description.volume 5 es_ES
dc.description.issue 9 es_ES
dc.relation.senia 254813 es_ES
dc.contributor.funder National Institute on Minority Health and Health Disparities es_ES
dc.contributor.funder Ministerio de Ciencia e Innovación es_ES
dc.contributor.funder National Institutes of Health es_ES
dc.contributor.funder National Science Foundation, EEUU es_ES
dc.contributor.funder Xunta de Galicia es_ES
dc.contributor.funder Consejo Superior de Investigaciones Científicas es_ES
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