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Direct synthesis of DME from syngas on hybrid CuZnAl/ZSM-5 catalysts: New insights into the role of zeolite acidity

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Direct synthesis of DME from syngas on hybrid CuZnAl/ZSM-5 catalysts: New insights into the role of zeolite acidity

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dc.contributor.author García Trenco, Andrés es_ES
dc.contributor.author Martinez Feliu, Agustin es_ES
dc.date.accessioned 2018-01-08T12:22:26Z
dc.date.available 2018-01-08T12:22:26Z
dc.date.issued 2012 es_ES
dc.identifier.issn 0926-860X es_ES
dc.identifier.uri http://hdl.handle.net/10251/94084
dc.description.abstract [EN] A commercial HZSM-5 zeolite (Si/Al = 16) was submitted to mild acid treatment and partial exchange of H+ by Na+ and Co2+ cations in order to produce samples with different amounts and strengths of Brensted and Lewis acid sites. The acid properties of the zeolites were determined by both FTIR of adsorbed pyridine and NH3-TPD. Then, hybrid catalysts comprising a CuO/ZnO/Al2O3 (CZA) methanol synthesis catalyst and the original and treated zeolites were prepared in order to analyze the impact of the zeolite acidity in the efficiency of the hybrids for the direct syngas-to-DME process. Independent methanol dehydration experiments on the bare zeolites and syngas-to-DME runs under methanol dehydration-controlled conditions were performed using hybrids with low zeolite concentration (CZA:zeolite mass ratio of 10:1) prepared by mixing the pre-pelletized CZA and zeolite components. The results revealed that both strong Bronsted and EFAL-related strong Lewis acid sites are the likely zeolite active sites for methanol dehydration at the typical syngas-to-DME temperature of 260 degrees C. Interestingly, we have found that different conclusions regarding the effect of zeolite acidity may be reached depending on the specific method used for preparing the hybrid catalysts when the overall syngas-to-DME process becomes controlled by the methanol synthesis rate on the Cu-based catalyst (i.e. using hybrids with a CZA:zeolite mass ratio of 2:1, that is, with an "excess" of acid sites). Thus, for hybrids prepared by mixing the pre-pelletized components, the same CO conversion and product selectivity (with values approaching those predicted by the thermodynamic equilibrium at the studied conditions) with no signs of deactivation during at least 50h on stream was attained irrespective of the zeolite acidity. By contrast, significant differences in catalyst stability were found for hybrids prepared by grinding the component powders prior to pelletizing. This fact points towards the occurrence of detrimental interactions between the CZA and zeolite components during the grinding preparation stage. The kind and extent of such detrimental interactions are tightly related to the properties (i.e. acidity, chemical composition) of the ZSM-5 zeolite. (C) 2011 Elsevier B.V. All rights reserved. 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 Ciencia e Innovación (MICINN) of Spain for a predoctoral (FPI) scholarship.
dc.language Inglés es_ES
dc.publisher Elsevier es_ES
dc.relation.ispartof Applied Catalysis A General 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 catalyst es_ES
dc.subject ZSM-5 es_ES
dc.subject Zeolite acidity es_ES
dc.title Direct synthesis of DME from syngas on hybrid CuZnAl/ZSM-5 catalysts: New insights into the role of zeolite acidity es_ES
dc.type Artículo es_ES
dc.identifier.doi 10.1016/j.apcata.2011.10.036 es_ES
dc.relation.projectID info:eu-repo/grantAgreement/MICINN//CTQ2010-17988/ES/CATALIZADORES AVANZADOS PARA LA CONVERSION DE GAS DE SINTESIS EN COMBUSTIBLES/
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. (2012). Direct synthesis of DME from syngas on hybrid CuZnAl/ZSM-5 catalysts: New insights into the role of zeolite acidity. Applied Catalysis A General. 411:170-179. https://doi.org/10.1016/j.apcata.2011.10.036 es_ES
dc.description.accrualMethod S es_ES
dc.relation.publisherversion https://doi.org/10.1016/j.apcata.2011.10.036 es_ES
dc.description.upvformatpinicio 170 es_ES
dc.description.upvformatpfin 179 es_ES
dc.type.version info:eu-repo/semantics/publishedVersion es_ES
dc.description.volume 411 es_ES
dc.relation.pasarela S\217762 es_ES
dc.contributor.funder Comisión Interministerial de Ciencia y Tecnología es_ES
dc.contributor.funder Ministerio de Ciencia e Innovación


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