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dc.contributor.author
Cored, Jorge
dc.contributor.author
Mazarío, Jaime
dc.contributor.author
Cerdá Moreno, Cristina
dc.contributor.author
Lustemberg, Pablo German
dc.contributor.author
Ganduglia Pirovano, M. Verónica
dc.contributor.author
Domine, Marcelo Eduardo
dc.contributor.author
Concepción, Patricia
dc.date.available
2023-08-24T14:29:13Z
dc.date.issued
2022-04
dc.identifier.citation
Cored, Jorge; Mazarío, Jaime; Cerdá Moreno, Cristina; Lustemberg, Pablo German; Ganduglia Pirovano, M. Verónica; et al.; Enhanced Methanol Production over Non-promoted Cu-MgO-Al2O3Materials with Ex-solved 2 nm Cu Particles: Insights from an Operando Spectroscopic Study; American Chemical Society; ACS Catalysis; 12; 7; 4-2022; 3845-3857
dc.identifier.issn
2155-5435
dc.identifier.uri
http://hdl.handle.net/11336/209257
dc.description.abstract
Enhanced methanol production is obtained over a non-promoted Cu-MgO-Al2O3 mixed oxide catalyst derived from a Cu-Mg-Al hydrotalcite precursor (HT) containing narrowly distributed small Cu NPs (2 nm). Conversions close to the equilibrium (∼20%) with a methanol selectivity of 67% are achieved at 230 °C, 20 bar, and a space velocity of 571 mL·gcat-1·h-1. Based on operando spectroscopic studies, the striking activity of this Cu-based catalyst is ascribed to the stabilization of Cu+ ions favored under reaction conditions due to lattice reorganization associated with the "HT-memory effect"promoted by water. Temperature-resolved infrared-mass spectrometry experiments have enabled the discernment of monodentate formate species, stabilized on Cu+ as the intermediate in methanol synthesis, in line with the results of density functional theory calculations. These monodentate formate species are much more reactive than bridge formate species, the latter ones behaving as intermediates in methane and CO formation. Moreover, poisoning of the Cu0 surface by strongly adsorbed species behaving as spectators is observed under reaction conditions. This work presents a detailed spectroscopic study highlighting the influence of the reaction pressure on the stabilization of active surface sites, and the possibility of enhancing methanol production on usually less active non-promoted nano-sized copper catalysts, provided that the proper support is selected, allowing the stabilization of doped Cu+. Thus, a methanol formation rate of 2.6 × 10-3 molMeOH·gcat-1·h-1 at 230 °C, 20 bar, and WHSV = 28 500 mL·gcat-1·h-1 is obtained on the Cu-MgO-Al2O3 HT-derived catalyst with 71% methanol selectivity, compared to 2.2 × 10-4 molMeOH·gcat-1·h-1 with 54% methanol selectivity obtained on a reference Cu/(Al2O3/MgO) catalyst not derived from a HT structure.
dc.format
application/pdf
dc.language.iso
eng
dc.publisher
American Chemical Society
dc.rights
info:eu-repo/semantics/openAccess
dc.rights.uri
https://creativecommons.org/licenses/by/2.5/ar/
dc.subject
CO2
dc.subject
COPPER
dc.subject
HYDROTALCITE
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IR SPECTROSCOPY
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METHANOL
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OPERANDO SPECTROSCOPY
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Otras Ciencias Químicas
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Ciencias Químicas
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CIENCIAS NATURALES Y EXACTAS
dc.title
Enhanced Methanol Production over Non-promoted Cu-MgO-Al2O3Materials with Ex-solved 2 nm Cu Particles: Insights from an Operando Spectroscopic Study
dc.type
info:eu-repo/semantics/article
dc.type
info:ar-repo/semantics/artículo
dc.type
info:eu-repo/semantics/publishedVersion
dc.date.updated
2023-07-17T17:49:52Z
dc.journal.volume
12
dc.journal.number
7
dc.journal.pagination
3845-3857
dc.journal.pais
Estados Unidos
dc.description.fil
Fil: Cored, Jorge. Consejo Superior de Investigaciones Científicas; España
dc.description.fil
Fil: Mazarío, Jaime. Consejo Superior de Investigaciones Científicas; España
dc.description.fil
Fil: Cerdá Moreno, Cristina. Consejo Superior de Investigaciones Científicas; España
dc.description.fil
Fil: Lustemberg, Pablo German. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; Argentina
dc.description.fil
Fil: Ganduglia Pirovano, M. Verónica. Consejo Superior de Investigaciones Científicas; España
dc.description.fil
Fil: Domine, Marcelo Eduardo. Consejo Superior de Investigaciones Científicas; España
dc.description.fil
Fil: Concepción, Patricia. Consejo Superior de Investigaciones Científicas; España
dc.journal.title
ACS Catalysis
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/doi/http://dx.doi.org/10.1021/acscatal.1c06044
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