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A heterogeneous mechanism for the catalytic decomposition of hydroperoxides and oxidation of alkanes over CeO2 nanoparticles: A combined theoretical and experimental study

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A heterogeneous mechanism for the catalytic decomposition of hydroperoxides and oxidation of alkanes over CeO2 nanoparticles: A combined theoretical and experimental study

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dc.contributor.author López Auséns, Javier Tirso es_ES
dc.contributor.author Boronat Zaragoza, Mercedes es_ES
dc.contributor.author Concepción Heydorn, Patricia es_ES
dc.contributor.author Chouzier, Sandra es_ES
dc.contributor.author Mastroianni, Sergio es_ES
dc.contributor.author Corma Canós, Avelino es_ES
dc.date.accessioned 2018-07-16T06:56:02Z
dc.date.available 2018-07-16T06:56:02Z
dc.date.issued 2016 es_ES
dc.identifier.issn 0021-9517 es_ES
dc.identifier.uri http://hdl.handle.net/10251/105846
dc.description.abstract [EN] A nanoparticulate CeO2 catalyst is presented that is able to oxidize cyclohexane to K/A-oil (a mixture of cyclohexanone and cyclohexanol) using hydroperoxides as oxidizing species. The improvement in selectivity with decreasing particle size suggests the existence of a structure-activity relationship in this process, and points to a preferential activation of cyclohexane at defective corner or edge sites. A detailed theoretical study of the reaction mechanism over three different CeO2 catalyst models shows that cyclohexane is preferentially activated by bicoordinated oxygen atoms present at the edges of small particles, following a Mars van Krevelen mechanism which has been confirmed by in situ IR spectroscopy and O-18/O-16 isotopic exchange experiments. The process is fully heterogeneous, and the catalyst can be reused without loss of activity up to four cycles. es_ES
dc.description.sponsorship The authors thank Solvay, MINECO (Consolider Ingenio 2010-MULTICAT, CSD2009-00050 and Severo Ochoa program, SEV-2012-0267), Generalitat Valenciana (PROMETEOII/2013/011 Project) and the European Union (ERC-AdG-2014-671093 - SynCat-Match) for financial support. Red Espanola de Supercomputacion (RES) and Centre de Calcul de la Universitat de Valencia are gratefully acknowledged for computational facilities and technical assistance. The technical support of the Electronic Microscopy Service of UPV is kindly appreciated. T.L.-A. thanks ITQ for a contract. We are grateful to Special Chem and Fabien Ocampo for providing ceria materials, and to Konstantin Neyman for providing the Ce<INF>21</INF>O<INF>42</INF> and Ce<INF>40</INF>O<INF>80</INF> nanoparticle models. en_EN
dc.language Inglés es_ES
dc.publisher Elsevier es_ES
dc.relation 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 MINECO/SEV-2012-0267 es_ES
dc.relation GV/PROMETEOII/2013/011 es_ES
dc.relation ERC/ERC-AdG-2014-671093 es_ES
dc.relation.ispartof Journal of Catalysis es_ES
dc.rights Reserva de todos los derechos es_ES
dc.subject Alkane oxidation es_ES
dc.subject Heterogeneous catalysis es_ES
dc.subject Acid-base es_ES
dc.subject Redox es_ES
dc.subject Ceria es_ES
dc.subject DFT es_ES
dc.subject in situ IR es_ES
dc.subject Electron Microscopy Service of the UPV
dc.subject.classification QUIMICA ORGANICA es_ES
dc.title A heterogeneous mechanism for the catalytic decomposition of hydroperoxides and oxidation of alkanes over CeO2 nanoparticles: A combined theoretical and experimental study es_ES
dc.type Artículo es_ES
dc.identifier.doi 10.1016/j.jcat.2016.09.032 es_ES
dc.relation.projectID info:eu-repo/grantAgreement/EC/H2020/671093/EU/MATching zeolite SYNthesis with CATalytic activity/ es_ES
dc.rights.accessRights Cerrado 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 López Auséns, JT.; Boronat Zaragoza, M.; Concepción Heydorn, P.; Chouzier, S.; Mastroianni, S.; Corma Canós, A. (2016). A heterogeneous mechanism for the catalytic decomposition of hydroperoxides and oxidation of alkanes over CeO2 nanoparticles: A combined theoretical and experimental study. Journal of Catalysis. 344:334-345. https://doi.org/10.1016/j.jcat.2016.09.032 es_ES
dc.description.accrualMethod S es_ES
dc.relation.publisherversion https://doi.org/10.1016/j.jcat.2016.09.032 es_ES
dc.description.upvformatpinicio 334 es_ES
dc.description.upvformatpfin 345 es_ES
dc.type.version info:eu-repo/semantics/publishedVersion es_ES
dc.description.volume 344 es_ES
dc.relation.pasarela S\328462 es_ES
dc.contributor.funder Ministerio de Ciencia e Innovación es_ES
dc.contributor.funder Generalitat Valenciana es_ES
dc.contributor.funder European Research Council es_ES
dc.contributor.funder Ministerio de Economía y Competitividad es_ES


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