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The influence of zeolite surface-aluminum species on the deactivationof CuZnAl/zeolite hybrid catalysts for the direct DME synthesis

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The influence of zeolite surface-aluminum species on the deactivationof CuZnAl/zeolite hybrid catalysts for the direct DME synthesis

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dc.contributor.author García Trenco, Andrés es_ES
dc.contributor.author Martinez Feliu, Agustin es_ES
dc.date.accessioned 2016-05-05T11:39:39Z
dc.date.available 2016-05-05T11:39:39Z
dc.date.issued 2014-05-15
dc.identifier.issn 0920-5861
dc.identifier.uri http://hdl.handle.net/10251/63696
dc.description.abstract [EN] The influence of the nature and amount of zeolite-surface Al species on the deactivation behavior ofbifunctional CZA/zeolite hybrid catalysts during the direct DME synthesis (260◦C, 4.0 MPa) from syn-gas (66% H2, 30% CO, 4% CO2) has been studied. To this aim, a series of delaminated ITQ-2 zeolites hasbeen prepared by acid treatment and steaming of an Al-ITQ-2 (Si/Al = 12) sample as well as by impreg-nation of an all-silica Si-ITQ-2 sample with Al(NO3)3(aq.) and calcination, and used as the methanoldehydration function of the hybrids. When prepared by grinding, all the hybrid catalysts experienced aloss of activity with time during the syngas-to-DME reaction under conditions where the synthesis ofmethanol on the copper catalyst (CZA) controlled the overall DME synthesis rate. The decay was neitherrelated to changes in the properties of the Cu species (dispersion, Cu0surface area) nor to depositionof carbon species on the metallic function (as ascertained by TPO) but to a particular mode of deacti-vation of the CZA catalyst due to adverse interactions between the copper component and the zeolite.Interestingly, the extent of the deactivation was seen to increase linearly with a parameter ˇ, arbitrarilydefined as ˇ = Sext× [Al/(Si + Al)]surf× %EFAL/100, where Sextis the external surface area of the zeolite,[Al/(Si + Al)]surfis the relative Al surface concentration (from XPS), and %EFAL is the percentage of penta-and hexacoordinated extraframework Al species with respect to the total Al detected by27Al MAS NMR.The correlation suggests that EFAL species located at the surface contact between the CZA and zeoliteparticles were primarily responsible for this particular mode of deactivation of the copper catalyst. Wehypothesize that EFAL species could migrate to the CZA catalyst during DME synthesis through a water-assisted mechanism, modifying the interaction between Cu and ZnOxat the Cu ZnOxinterface where theactive copper sites are likely located es_ES
dc.description.sponsorship Financial support by the Comisión Interministerial de Ciencia y Tecnología (CICYT) of Spain through the Project CTQ2010-17988/PPQ is gratefully acknowledged. A. García-Trenco thanks the Ministerio de Economía y Competitividad (former Ministerio de Ciencia e Innovación) of Spain for a predoctoral (FPI) scholarship.
dc.language Inglés es_ES
dc.publisher Elsevier es_ES
dc.relation.ispartof Catalysis Today es_ES
dc.rights Reserva de todos los derechos es_ES
dc.subject Synthesis gas es_ES
dc.subject Direct DME synthesis es_ES
dc.subject CuZnAl methanol synthesis catalyst es_ES
dc.subject ITQ-2 zeolite es_ES
dc.subject Deactivation es_ES
dc.subject Hybrid catalysts es_ES
dc.title The influence of zeolite surface-aluminum species on the deactivationof CuZnAl/zeolite hybrid catalysts for the direct DME synthesis es_ES
dc.type Artículo es_ES
dc.identifier.doi 10.1016/j.cattod.2013.09.051
dc.relation.projectID info:eu-repo/grantAgreement/MICINN//CTQ2010-17988/ES/CATALIZADORES AVANZADOS PARA LA CONVERSION DE GAS DE SINTESIS EN COMBUSTIBLES/ 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.description.bibliographicCitation García Trenco, A.; Martinez Feliu, A. (2014). The influence of zeolite surface-aluminum species on the deactivationof CuZnAl/zeolite hybrid catalysts for the direct DME synthesis. Catalysis Today. 227:144-153. https://doi.org/10.1016/j.cattod.2013.09.051 es_ES
dc.description.accrualMethod S es_ES
dc.relation.publisherversion http://dx.doi.org/10.1016/j.cattod.2013.09.051 es_ES
dc.description.upvformatpinicio 144 es_ES
dc.description.upvformatpfin 153 es_ES
dc.type.version info:eu-repo/semantics/publishedVersion es_ES
dc.description.volume 227 es_ES
dc.relation.senia 286642 es_ES
dc.contributor.funder Ministerio de Ciencia e Innovación


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