Selective detection of reaction intermediates using concentration-modulation excitation DRIFT spectroscopy

Autores
Aguirre, Alejo; Collins, Sebastián Enrique
Año de publicación
2013
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Concentration-modulation excitation spectroscopy (MES) experiments in combination with phase-sensitive detection (PSD) were used to monitor the gas–solid interface by means of in operando diffuse reflectance infrared spectroscopy (DRIFT). The MES methodology is a powerful technique because it allows sensitive and selective spectroscopic detection and monitoring of the dynamic behavior of species directly involved in a reaction. In this work, c-MES was employed to monitor the adsorption of hydrogen and carbon dioxide and their reaction (reverse water gas shift) on a model Pd(1 wt.%)/γ-Ga2O3catalyst. Details of the reaction mechanism could be reached: (i) H2 is dissociatively chemisorbed on the gallium oxide surface giving Ga–H species; (ii) CO2 is adsorbed giving rise of carbonate groups; (iii) on the gallia surface, carbonates are hydrogenated by Ga–H to produce formate species with different coordination, e.g. monodentate, bidentate and bridged formates, which in turn are decomposed into CO(g); (iv) the metal phase increases the formate surface concentration onto the gallia because of an efficient supply of atomic hydrogen via a spillover. Results also indicated that monodentate formates are the most reactive intermediate.
Fil: Aguirre, Alejo. 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
Fil: Collins, Sebastián Enrique. 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
Materia
DRIFT
FORMATES
MODULATION EXCITATION SPECTROSCOPY
PALLADIUM-GALLIA
REVERSE WATER GAS SHIFT REACTION
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:11336/1988
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/1988
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Selective detection of reaction intermediates using concentration-modulation excitation DRIFT spectroscopyAguirre, AlejoCollins, Sebastián EnriqueDRIFTFORMATESMODULATION EXCITATION SPECTROSCOPYPALLADIUM-GALLIAREVERSE WATER GAS SHIFT REACTIONhttps://purl.org/becyt/ford/2.4https://purl.org/becyt/ford/2Concentration-modulation excitation spectroscopy (MES) experiments in combination with phase-sensitive detection (PSD) were used to monitor the gas–solid interface by means of in operando diffuse reflectance infrared spectroscopy (DRIFT). The MES methodology is a powerful technique because it allows sensitive and selective spectroscopic detection and monitoring of the dynamic behavior of species directly involved in a reaction. In this work, c-MES was employed to monitor the adsorption of hydrogen and carbon dioxide and their reaction (reverse water gas shift) on a model Pd(1 wt.%)/γ-Ga2O3catalyst. Details of the reaction mechanism could be reached: (i) H2 is dissociatively chemisorbed on the gallium oxide surface giving Ga–H species; (ii) CO2 is adsorbed giving rise of carbonate groups; (iii) on the gallia surface, carbonates are hydrogenated by Ga–H to produce formate species with different coordination, e.g. monodentate, bidentate and bridged formates, which in turn are decomposed into CO(g); (iv) the metal phase increases the formate surface concentration onto the gallia because of an efficient supply of atomic hydrogen via a spillover. Results also indicated that monodentate formates are the most reactive intermediate.Fil: Aguirre, Alejo. 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; ArgentinaFil: Collins, Sebastián Enrique. 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; ArgentinaElsevier Science2013-04-30info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/1988Aguirre, Alejo; Collins, Sebastián Enrique; Selective detection of reaction intermediates using concentration-modulation excitation DRIFT spectroscopy; Elsevier Science; Catalysis Today; 205; 30-4-2013; 34-400920-5861eng4th International Congress on Operando Spectroscopyinfo:eu-repo/semantics/altIdentifier/url/http://www.sciencedirect.com/science/article/pii/S0920586112005895info:eu-repo/semantics/altIdentifier/doi/10.1016/j.cattod.2012.08.020info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T09:47:09Zoai:ri.conicet.gov.ar:11336/1988instacron: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 09:47:10.117CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Selective detection of reaction intermediates using concentration-modulation excitation DRIFT spectroscopy
title Selective detection of reaction intermediates using concentration-modulation excitation DRIFT spectroscopy
spellingShingle Selective detection of reaction intermediates using concentration-modulation excitation DRIFT spectroscopy
Aguirre, Alejo
DRIFT
FORMATES
MODULATION EXCITATION SPECTROSCOPY
PALLADIUM-GALLIA
REVERSE WATER GAS SHIFT REACTION
title_short Selective detection of reaction intermediates using concentration-modulation excitation DRIFT spectroscopy
title_full Selective detection of reaction intermediates using concentration-modulation excitation DRIFT spectroscopy
title_fullStr Selective detection of reaction intermediates using concentration-modulation excitation DRIFT spectroscopy
title_full_unstemmed Selective detection of reaction intermediates using concentration-modulation excitation DRIFT spectroscopy
title_sort Selective detection of reaction intermediates using concentration-modulation excitation DRIFT spectroscopy
dc.creator.none.fl_str_mv Aguirre, Alejo
Collins, Sebastián Enrique
author Aguirre, Alejo
author_facet Aguirre, Alejo
Collins, Sebastián Enrique
author_role author
author2 Collins, Sebastián Enrique
author2_role author
dc.subject.none.fl_str_mv DRIFT
FORMATES
MODULATION EXCITATION SPECTROSCOPY
PALLADIUM-GALLIA
REVERSE WATER GAS SHIFT REACTION
topic DRIFT
FORMATES
MODULATION EXCITATION SPECTROSCOPY
PALLADIUM-GALLIA
REVERSE WATER GAS SHIFT REACTION
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.4
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv Concentration-modulation excitation spectroscopy (MES) experiments in combination with phase-sensitive detection (PSD) were used to monitor the gas–solid interface by means of in operando diffuse reflectance infrared spectroscopy (DRIFT). The MES methodology is a powerful technique because it allows sensitive and selective spectroscopic detection and monitoring of the dynamic behavior of species directly involved in a reaction. In this work, c-MES was employed to monitor the adsorption of hydrogen and carbon dioxide and their reaction (reverse water gas shift) on a model Pd(1 wt.%)/γ-Ga2O3catalyst. Details of the reaction mechanism could be reached: (i) H2 is dissociatively chemisorbed on the gallium oxide surface giving Ga–H species; (ii) CO2 is adsorbed giving rise of carbonate groups; (iii) on the gallia surface, carbonates are hydrogenated by Ga–H to produce formate species with different coordination, e.g. monodentate, bidentate and bridged formates, which in turn are decomposed into CO(g); (iv) the metal phase increases the formate surface concentration onto the gallia because of an efficient supply of atomic hydrogen via a spillover. Results also indicated that monodentate formates are the most reactive intermediate.
Fil: Aguirre, Alejo. 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
Fil: Collins, Sebastián Enrique. 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
description Concentration-modulation excitation spectroscopy (MES) experiments in combination with phase-sensitive detection (PSD) were used to monitor the gas–solid interface by means of in operando diffuse reflectance infrared spectroscopy (DRIFT). The MES methodology is a powerful technique because it allows sensitive and selective spectroscopic detection and monitoring of the dynamic behavior of species directly involved in a reaction. In this work, c-MES was employed to monitor the adsorption of hydrogen and carbon dioxide and their reaction (reverse water gas shift) on a model Pd(1 wt.%)/γ-Ga2O3catalyst. Details of the reaction mechanism could be reached: (i) H2 is dissociatively chemisorbed on the gallium oxide surface giving Ga–H species; (ii) CO2 is adsorbed giving rise of carbonate groups; (iii) on the gallia surface, carbonates are hydrogenated by Ga–H to produce formate species with different coordination, e.g. monodentate, bidentate and bridged formates, which in turn are decomposed into CO(g); (iv) the metal phase increases the formate surface concentration onto the gallia because of an efficient supply of atomic hydrogen via a spillover. Results also indicated that monodentate formates are the most reactive intermediate.
publishDate 2013
dc.date.none.fl_str_mv 2013-04-30
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/11336/1988
Aguirre, Alejo; Collins, Sebastián Enrique; Selective detection of reaction intermediates using concentration-modulation excitation DRIFT spectroscopy; Elsevier Science; Catalysis Today; 205; 30-4-2013; 34-40
0920-5861
url http://hdl.handle.net/11336/1988
identifier_str_mv Aguirre, Alejo; Collins, Sebastián Enrique; Selective detection of reaction intermediates using concentration-modulation excitation DRIFT spectroscopy; Elsevier Science; Catalysis Today; 205; 30-4-2013; 34-40
0920-5861
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv 4th International Congress on Operando Spectroscopy
info:eu-repo/semantics/altIdentifier/url/http://www.sciencedirect.com/science/article/pii/S0920586112005895
info:eu-repo/semantics/altIdentifier/doi/10.1016/j.cattod.2012.08.020
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 Science
publisher.none.fl_str_mv Elsevier Science
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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score 13.070432

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