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A simple an efficient approach to confine Cu/ZnO methanol synthesis catalysts in the ordered mesoporous SBA-15 silica

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A simple an efficient approach to confine Cu/ZnO methanol synthesis catalysts in the ordered mesoporous SBA-15 silica

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dc.contributor.author García Trenco, Andrés es_ES
dc.contributor.author Martinez Feliu, Agustin es_ES
dc.date.accessioned 2015-06-16T11:32:21Z
dc.date.issued 2013-10-15
dc.identifier.issn 0920-5861
dc.identifier.uri http://hdl.handle.net/10251/51780
dc.description.abstract The ammonia-driving deposition-precipitation (ADP) method has been applied with the purpose of confining active Cu/ZnO methanol synthesis phases inside the pores of the ordered mesoporous SBA-15 silica. Thus, a series of CuZnx/SBA-15 catalysts with total (Cu + Zn) metal loading of 35 wt% and Cu/Zn mass ratios (x) of 0.5, 1, 2, 4, and 6, as well as a Zn-free Cu/SBA-15 sample, have been prepared. Additionally, a CuZn2/SBA-15 sample (Cu + Zn = 35 wt%, Cu/Zn = 2) prepared by impregnation and a coprecipitated Cu-ZnO-Al2O3 (CZA) catalyst have been prepared as reference. The materials have been characterized by ICP-OES, N2 physisorption, XRD, in situ H2-XRD, TEM, H2-TPR, and N2O chemisorption, and their methanol synthesis activities determined, after in situ H2 reduction, under realistic conditions (533 K, 4.0 MPa, syngas: 66%/30%CO/4%CO2). Copper NPs in CuZnx/SBA-15 (ADP) catalysts with Cu/Zn mass ratios up to 2 were effectively confined within the SBA-15 pores (dCu < 7 nm) while at higher ratios part of Cu formed large particles sizing about 60¿70 nm on the external SBA-15 surface. Similar large Cu NPs were also found for the impregnated catalyst (Cu/Zn = 2). A maximum in the methanol synthesis activity was attained for the catalyst prepared by ADP with Cu/Zn mass ratio of 2. This catalyst displayed a synthesis activity about 14 times higher than the impregnated sample with equal composition and nearly the same activity (per mass of Cu) than the reference CZA catalyst. No direct relationship between the methanol synthesis rate and Cu0 surface area was found for the studied catalysts. Instead, our results strongly suggested that the active sites are located at the Cu0-ZnOx interface, which can be maximized through the effective confinement of Cu0 NPs inside the SBA-15 channels using the simple ADP method. es_ES
dc.description.sponsorship Financial support by the Comision Interministerial de Ciencia y Tecnologia (CICYT) of Spain through the Project CTQ2010-17988/PPQ is gratefully acknowledged. Thanks are also due to Dr. J.L. Jorda (ITQ), for performing the in situ H<INF>2</INF>-XRD experiments. A. Garcia-Trenco thanks the Ministerio de Economia y Competitividad (former Ministerio de Ciencia e Innovacion) of Spain for a predoctoral (FPI) scholarship. en_EN
dc.language Inglés es_ES
dc.publisher Elsevier es_ES
dc.relation Comisión Interministerial de Ciencia y Tecnología (CICYT) CTQ2010- 17988/PPQ 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 Methanol synthesis es_ES
dc.subject Copper nanoparticles es_ES
dc.subject Cu/ZnO catalyst es_ES
dc.subject Confined catalyst es_ES
dc.subject Mesoporous silica es_ES
dc.subject SBA-15 es_ES
dc.title A simple an efficient approach to confine Cu/ZnO methanol synthesis catalysts in the ordered mesoporous SBA-15 silica es_ES
dc.type Artículo es_ES
dc.embargo.lift 10000-01-01
dc.embargo.terms forever es_ES
dc.identifier.doi 10.1016/j.cattod.2013.03.005
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.description.bibliographicCitation García Trenco, A.; Martinez Feliu, A. (2013). A simple an efficient approach to confine Cu/ZnO methanol synthesis catalysts in the ordered mesoporous SBA-15 silica. Catalysis Today. 215:152-161. doi:10.1016/j.cattod.2013.03.005 es_ES
dc.description.accrualMethod Senia es_ES
dc.relation.publisherversion http://dx.doi.org/10.1016/j.cattod.2013.03.005 es_ES
dc.description.upvformatpinicio 152 es_ES
dc.description.upvformatpfin 161 es_ES
dc.type.version info:eu repo/semantics/publishedVersion es_ES
dc.description.volume 215 es_ES
dc.relation.senia 248521


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