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dc.contributor.author
Fornero, Esteban Luis
dc.contributor.author
Bonivardi, Adrian Lionel
dc.contributor.author
Baltanas, Miguel Angel
dc.date.available
2017-08-25T21:44:05Z
dc.date.issued
2015-08
dc.identifier.citation
Fornero, Esteban Luis; Bonivardi, Adrian Lionel; Baltanas, Miguel Angel; Isotopic study of the rates of hydrogen provision vs. methanol synthesis from CO2 over Cu-Ga-Zr catalysts; Academic Press Inc Elsevier Science; Journal of Catalysis; 330; 8-2015; 302-310
dc.identifier.issn
0021-9517
dc.identifier.uri
http://hdl.handle.net/11336/23075
dc.description.abstract
Cu/ZrO2 and Ga2O3-promoted Cu/ZrO2, with the same copper loading (2.6 wt.%), were evaluated in a Carberry-type batch-operated microreactor for methanol synthesis using a H2/CO2/He mixture (75/22/3 v/v) at 1.6 MPa and 498 K. The gallia-promoted catalyst was 5-fold more active to methanol production (per catalyst specific surface) than Cu/ZrO2. In addition, after the incorporation of Ga2O3 the selectivity to the alcohol was enhanced by a factor of three. To discern whether different degrees of hydrogen provision were responsible for the dissimilar performances observed, thus affecting the overall reaction rate to methanol (RCH3OH), the ability to activate H2 of the catalysts was assessed – in the same microreactor – by a combination of H2/D2 isotopic equilibration (H2/D2/Ar = 37.5/37.5/25 v/v) and H/D isotopic exchange (D2/Ar = 10/90 v/v) reactions at 0.1 MPa, between 353 and 393 K. The equilibration rate (Requil) was far higher than RCH3OH on both, Cu/ZrO2 and Ga2O3-promoted Cu/ZrO2. In agreement with the property of gallia to dissociate H2, Ga2O3 increased further Requil in the ternary catalyst. Vis-à-vis, the isotopic-exchange reaction rates (Rexchg) were considerably lower than the Requil for each catalyst, more so for the gallium containing one. However, the extrapolation of those Rexchg values to the temperature of methanol synthesis gave always much higher rates than RCH3OH, thus allowing to conclude that the supply of ‘active’ hydrogen is fully secured on these copper-supported (gallium-promoted) catalysts.
dc.format
application/pdf
dc.language.iso
eng
dc.publisher
Academic Press Inc Elsevier Science
dc.rights
info:eu-repo/semantics/openAccess
dc.rights.uri
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.subject
Methanol Synthesis
dc.subject
Hydrogen Provision
dc.subject
Copper
dc.subject
Zirconia
dc.subject
Galia
dc.subject.classification
Otras Ingeniería Química
dc.subject.classification
Ingeniería Química
dc.subject.classification
INGENIERÍAS Y TECNOLOGÍAS
dc.title
Isotopic study of the rates of hydrogen provision vs. methanol synthesis from CO2 over Cu-Ga-Zr catalysts
dc.type
info:eu-repo/semantics/article
dc.type
info:ar-repo/semantics/artículo
dc.type
info:eu-repo/semantics/publishedVersion
dc.date.updated
2017-08-17T13:44:03Z
dc.journal.volume
330
dc.journal.pagination
302-310
dc.journal.pais
Países Bajos
dc.journal.ciudad
Amsterdam
dc.description.fil
Fil: Fornero, Esteban Luis. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Desarrollo Tecnológico para la Industria Química. Universidad Nacional del Litoral. Instituto de Desarrollo Tecnológico para la Industria Química; Argentina
dc.description.fil
Fil: Bonivardi, Adrian Lionel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Desarrollo Tecnológico para la Industria Química. Universidad Nacional del Litoral. Instituto de Desarrollo Tecnológico para la Industria Química; Argentina
dc.description.fil
Fil: Baltanas, Miguel Angel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Desarrollo Tecnológico para la Industria Química. Universidad Nacional del Litoral. Instituto de Desarrollo Tecnológico para la Industria Química; Argentina
dc.journal.title
Journal of Catalysis
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/doi/http://dx.doi.org/10.1016/j.jcat.2015.07.025
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/url/http://www.sciencedirect.com/science/article/pii/S0021951715002456
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