Deactivation of Cu–Mg–Al mixed oxide catalysts for liquid transportation fuel synthesis from biomass-derived resources

Autores
Luggren, Pablo Jorge; Di Cosimo, Juana Isabel
Año de publicación
2018
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
A “platform molecule” (2-hexanol) obtained from the primary conversion of sugars was upgraded to liquid transportation fuel precursors under gas phase conditions at 573 K and 101.3 kPa. Reaction was promoted by Cu-Mg-Al mixed oxides with different copper loading (0.3–61.2%) and a Mg/Al = 1.5 (molar ratio). Products were mainly low oxygen content C9-C24 oxygenates and hydrocarbons. The product pool average molecular weight and the oxygenates/hydrocarbons ratio increase with the catalyst copper loading, but the latter might be diminished by augmenting the contact time. A slow catalyst deactivation process occurs in the first 2 h of reaction. Temperature-programmed oxidation, BET surface are measurements and X-ray photoelectron and Auger electron spectroscopies of the spent catalysts indicated that the main reasons for the activity decay during reaction are carbon deposition on the active sites and, to a lesser degree, partial oxidation of the surface copper particles. Oxygenates (reactant or products) are the chemical species responsible for deactivation. The initial deactivation rate (rd0) depends on the copper content and contact time. On catalysts with low Cu content, rd0 is higher at short contact times, which is consistent with coke formed directly from the reactant. Contrarily, at high Cu loadings rd0 increases with contact time and parallels formation of heavy unsaturated oxygenates. Oxidation/reduction/catalytic test cycles of spent Cu-Mg-Al mixed oxides were implemented to explore catalyst reusability.
Fil: Luggren, Pablo Jorge. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; Argentina
Fil: Di Cosimo, Juana Isabel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; Argentina
Materia
2-HEXANOL
ALDOL CONDENSATION
CU-MG-AL MIXED OXIDES
DEACTIVATION
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/88469

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spelling Deactivation of Cu–Mg–Al mixed oxide catalysts for liquid transportation fuel synthesis from biomass-derived resourcesLuggren, Pablo JorgeDi Cosimo, Juana Isabel2-HEXANOLALDOL CONDENSATIONCU-MG-AL MIXED OXIDESDEACTIVATIONhttps://purl.org/becyt/ford/2.4https://purl.org/becyt/ford/2A “platform molecule” (2-hexanol) obtained from the primary conversion of sugars was upgraded to liquid transportation fuel precursors under gas phase conditions at 573 K and 101.3 kPa. Reaction was promoted by Cu-Mg-Al mixed oxides with different copper loading (0.3–61.2%) and a Mg/Al = 1.5 (molar ratio). Products were mainly low oxygen content C9-C24 oxygenates and hydrocarbons. The product pool average molecular weight and the oxygenates/hydrocarbons ratio increase with the catalyst copper loading, but the latter might be diminished by augmenting the contact time. A slow catalyst deactivation process occurs in the first 2 h of reaction. Temperature-programmed oxidation, BET surface are measurements and X-ray photoelectron and Auger electron spectroscopies of the spent catalysts indicated that the main reasons for the activity decay during reaction are carbon deposition on the active sites and, to a lesser degree, partial oxidation of the surface copper particles. Oxygenates (reactant or products) are the chemical species responsible for deactivation. The initial deactivation rate (rd0) depends on the copper content and contact time. On catalysts with low Cu content, rd0 is higher at short contact times, which is consistent with coke formed directly from the reactant. Contrarily, at high Cu loadings rd0 increases with contact time and parallels formation of heavy unsaturated oxygenates. Oxidation/reduction/catalytic test cycles of spent Cu-Mg-Al mixed oxides were implemented to explore catalyst reusability.Fil: Luggren, Pablo Jorge. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; ArgentinaFil: Di Cosimo, Juana Isabel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; ArgentinaElsevier B.V.2018-08info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/88469Luggren, Pablo Jorge; Di Cosimo, Juana Isabel; Deactivation of Cu–Mg–Al mixed oxide catalysts for liquid transportation fuel synthesis from biomass-derived resources; Elsevier B.V.; Molecular Catalysis; 8-2018; 1-112468-8231CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://linkinghub.elsevier.com/retrieve/pii/S2468823118303250info:eu-repo/semantics/altIdentifier/doi/10.1016/j.mcat.2018.08.008info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T09:45:17Zoai:ri.conicet.gov.ar:11336/88469instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-09-29 09:45:17.377CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Deactivation of Cu–Mg–Al mixed oxide catalysts for liquid transportation fuel synthesis from biomass-derived resources
title Deactivation of Cu–Mg–Al mixed oxide catalysts for liquid transportation fuel synthesis from biomass-derived resources
spellingShingle Deactivation of Cu–Mg–Al mixed oxide catalysts for liquid transportation fuel synthesis from biomass-derived resources
Luggren, Pablo Jorge
2-HEXANOL
ALDOL CONDENSATION
CU-MG-AL MIXED OXIDES
DEACTIVATION
title_short Deactivation of Cu–Mg–Al mixed oxide catalysts for liquid transportation fuel synthesis from biomass-derived resources
title_full Deactivation of Cu–Mg–Al mixed oxide catalysts for liquid transportation fuel synthesis from biomass-derived resources
title_fullStr Deactivation of Cu–Mg–Al mixed oxide catalysts for liquid transportation fuel synthesis from biomass-derived resources
title_full_unstemmed Deactivation of Cu–Mg–Al mixed oxide catalysts for liquid transportation fuel synthesis from biomass-derived resources
title_sort Deactivation of Cu–Mg–Al mixed oxide catalysts for liquid transportation fuel synthesis from biomass-derived resources
dc.creator.none.fl_str_mv Luggren, Pablo Jorge
Di Cosimo, Juana Isabel
author Luggren, Pablo Jorge
author_facet Luggren, Pablo Jorge
Di Cosimo, Juana Isabel
author_role author
author2 Di Cosimo, Juana Isabel
author2_role author
dc.subject.none.fl_str_mv 2-HEXANOL
ALDOL CONDENSATION
CU-MG-AL MIXED OXIDES
DEACTIVATION
topic 2-HEXANOL
ALDOL CONDENSATION
CU-MG-AL MIXED OXIDES
DEACTIVATION
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.4
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv A “platform molecule” (2-hexanol) obtained from the primary conversion of sugars was upgraded to liquid transportation fuel precursors under gas phase conditions at 573 K and 101.3 kPa. Reaction was promoted by Cu-Mg-Al mixed oxides with different copper loading (0.3–61.2%) and a Mg/Al = 1.5 (molar ratio). Products were mainly low oxygen content C9-C24 oxygenates and hydrocarbons. The product pool average molecular weight and the oxygenates/hydrocarbons ratio increase with the catalyst copper loading, but the latter might be diminished by augmenting the contact time. A slow catalyst deactivation process occurs in the first 2 h of reaction. Temperature-programmed oxidation, BET surface are measurements and X-ray photoelectron and Auger electron spectroscopies of the spent catalysts indicated that the main reasons for the activity decay during reaction are carbon deposition on the active sites and, to a lesser degree, partial oxidation of the surface copper particles. Oxygenates (reactant or products) are the chemical species responsible for deactivation. The initial deactivation rate (rd0) depends on the copper content and contact time. On catalysts with low Cu content, rd0 is higher at short contact times, which is consistent with coke formed directly from the reactant. Contrarily, at high Cu loadings rd0 increases with contact time and parallels formation of heavy unsaturated oxygenates. Oxidation/reduction/catalytic test cycles of spent Cu-Mg-Al mixed oxides were implemented to explore catalyst reusability.
Fil: Luggren, Pablo Jorge. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; Argentina
Fil: Di Cosimo, Juana Isabel. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones en Catálisis y Petroquímica "Ing. José Miguel Parera"; Argentina
description A “platform molecule” (2-hexanol) obtained from the primary conversion of sugars was upgraded to liquid transportation fuel precursors under gas phase conditions at 573 K and 101.3 kPa. Reaction was promoted by Cu-Mg-Al mixed oxides with different copper loading (0.3–61.2%) and a Mg/Al = 1.5 (molar ratio). Products were mainly low oxygen content C9-C24 oxygenates and hydrocarbons. The product pool average molecular weight and the oxygenates/hydrocarbons ratio increase with the catalyst copper loading, but the latter might be diminished by augmenting the contact time. A slow catalyst deactivation process occurs in the first 2 h of reaction. Temperature-programmed oxidation, BET surface are measurements and X-ray photoelectron and Auger electron spectroscopies of the spent catalysts indicated that the main reasons for the activity decay during reaction are carbon deposition on the active sites and, to a lesser degree, partial oxidation of the surface copper particles. Oxygenates (reactant or products) are the chemical species responsible for deactivation. The initial deactivation rate (rd0) depends on the copper content and contact time. On catalysts with low Cu content, rd0 is higher at short contact times, which is consistent with coke formed directly from the reactant. Contrarily, at high Cu loadings rd0 increases with contact time and parallels formation of heavy unsaturated oxygenates. Oxidation/reduction/catalytic test cycles of spent Cu-Mg-Al mixed oxides were implemented to explore catalyst reusability.
publishDate 2018
dc.date.none.fl_str_mv 2018-08
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/88469
Luggren, Pablo Jorge; Di Cosimo, Juana Isabel; Deactivation of Cu–Mg–Al mixed oxide catalysts for liquid transportation fuel synthesis from biomass-derived resources; Elsevier B.V.; Molecular Catalysis; 8-2018; 1-11
2468-8231
CONICET Digital
CONICET
url http://hdl.handle.net/11336/88469
identifier_str_mv Luggren, Pablo Jorge; Di Cosimo, Juana Isabel; Deactivation of Cu–Mg–Al mixed oxide catalysts for liquid transportation fuel synthesis from biomass-derived resources; Elsevier B.V.; Molecular Catalysis; 8-2018; 1-11
2468-8231
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/https://linkinghub.elsevier.com/retrieve/pii/S2468823118303250
info:eu-repo/semantics/altIdentifier/doi/10.1016/j.mcat.2018.08.008
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv Elsevier B.V.
publisher.none.fl_str_mv Elsevier B.V.
dc.source.none.fl_str_mv reponame:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
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