- -

Evidence of a Cu2+-Alkane Interaction in Cu-Zeolite Catalysts Crucial for the Selective Catalytic Reduction of NO with Hydrocarbons

RiuNet: Institutional repository of the Polithecnic University of Valencia

Share/Send to

Cited by

Statistics

  • Estadisticas de Uso

Evidence of a Cu2+-Alkane Interaction in Cu-Zeolite Catalysts Crucial for the Selective Catalytic Reduction of NO with Hydrocarbons

Show simple item record

Files in this item

dc.contributor.author Moreno González, Marta es_ES
dc.contributor.author Palomares Gimeno, Antonio Eduardo es_ES
dc.contributor.author Chiesa, Mario es_ES
dc.contributor.author Boronat Zaragoza, Mercedes es_ES
dc.contributor.author Giamello, Elio es_ES
dc.contributor.author Blasco Lanzuela, Teresa es_ES
dc.date.accessioned 2018-09-17T07:35:38Z
dc.date.available 2018-09-17T07:35:38Z
dc.date.issued 2017 es_ES
dc.identifier.issn 2155-5435 es_ES
dc.identifier.uri http://hdl.handle.net/10251/107407
dc.description.abstract [EN] The selective catalytic reduction of NOx with hydrocarbons (HC-SCR-NOx) on Cu-zeolites is an alternative for the depletion of NOx present in the exhaust gas of diesel engines. The role played by copper and the general reaction pathway are investigated here using propane as reductant (C3H8-SCR-NOx) and Cu-TNU-9 and Cu-Y zeolites as catalysts, giving 80% and 10% NO conversion, respectively, at 623 K. In situ EPR shows that, even at room temperature, Cu2+NO3- is with C3H8 in Cu-TNU-9 but not in Cu-Y. The formation of Cu2+---C3H8 formed in the two Cu-zeolites and that there exists an interaction of Cu2+ species in Cu-TNU-9 is confirmed by HYSCORE EPR experiments and theoretical calculations. Cu2+ is reduced to Cu+ after heating with the reaction mixture to an extent that is related with the catalyst activity. In situ NMR spectra have allowed identifying nitrile and isocyanate as reaction intermediates, which are partially hydrolyzed to carboxylic acid and ammonia. The results allow concluding that the C3H8-SCR-NOx reaction requires the activation of the alkane at accessible isolated Cu2+ and that this generates ammonia which reacts with Cu2+NO3- and NO acting as the reductant. The low activity of Cu-Y zeolite for the C3H8-SCR-NOx reaction proves that C3H8 in the gas phase does not react with Cu2+NO3-, the activation of C3H8 being mandatory on accessible Cu2+ sites. A general reaction scheme for HC-SCR-NOx involving Cu2+/Cu+ redox cycles and the formation of ammonia that acts as a reductant of NO is proposed. es_ES
dc.description.sponsorship The authors acknowledge financial support by the Spanish Government-MINECO through CTQ2015-68951-C3-1-R, "Severo Ochoa" (SEV 2012-0267), and the CSIC (i-Link0821). Red Espanola de Supercomputacion (RES) and Centre de Calcul de la Universitat de Valencia are gratefully acknowledged for computational facilities and technical assistance. M.M.-G. thanks the ITQ for grants. es_ES
dc.language Inglés es_ES
dc.publisher American Chemical Society es_ES
dc.relation.ispartof ACS Catalysis es_ES
dc.rights Reserva de todos los derechos es_ES
dc.subject SCR-NOx es_ES
dc.subject Hydrocarbons es_ES
dc.subject Propane es_ES
dc.subject EPR es_ES
dc.subject NMR es_ES
dc.subject HYSCORE es_ES
dc.subject Cu-zeolite es_ES
dc.subject.classification INGENIERIA QUIMICA es_ES
dc.title Evidence of a Cu2+-Alkane Interaction in Cu-Zeolite Catalysts Crucial for the Selective Catalytic Reduction of NO with Hydrocarbons es_ES
dc.type Artículo es_ES
dc.identifier.doi 10.1021/acscatal.6b03473 es_ES
dc.relation.projectID info:eu-repo/grantAgreement/MINECO//CTQ2015-68951-C3-1-R/ES/TRATAMIENTOS CATALITICOS AVANZADOS PARA LA VALORIZACION DE LA BIOMASA Y LA ELIMINACION DE RESIDUOS ASOCIADOS/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/MINECO//SEV-2012-0267/
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 Ingeniería Química y Nuclear - Departament d'Enginyeria Química i Nuclear es_ES
dc.description.bibliographicCitation Moreno González, M.; Palomares Gimeno, AE.; Chiesa, M.; Boronat Zaragoza, M.; Giamello, E.; Blasco Lanzuela, T. (2017). Evidence of a Cu2+-Alkane Interaction in Cu-Zeolite Catalysts Crucial for the Selective Catalytic Reduction of NO with Hydrocarbons. ACS Catalysis. 7(5):3501-3509. https://doi.org/10.1021/acscatal.6b03473 es_ES
dc.description.accrualMethod S es_ES
dc.relation.publisherversion http://doi.org/10.1021/acscatal.6b03473 es_ES
dc.description.upvformatpinicio 3501 es_ES
dc.description.upvformatpfin 3509 es_ES
dc.type.version info:eu-repo/semantics/publishedVersion es_ES
dc.description.volume 7 es_ES
dc.description.issue 5 es_ES
dc.relation.pasarela S\346739 es_ES
dc.contributor.funder Ministerio de Economía y Competitividad es_ES


This item appears in the following Collection(s)

Show simple item record