NO reduction with CO in the presence and absence of H2O over Pd/γ-Al2O3 and Pd-VOx/γ-Al2O3 catalysts: The formation of HNCO, NH3 and stable surface species

Autores
Neyertz, Claudia A.; Volpe, María Alicia; Perez, D.; Costilla, Ignacio Oscar; Sanchez, Miguel Dario; Gigola, Carlos Eugenio
Año de publicación
2009
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The reduction of NO by CO over Pd/γ-Al2O3 and Pd-VOx/γ-Al2O3 catalysts has been studied by combining activity and selectivity measurements with FTIR spectroscopy of gas phase products and adsorbed species under reaction conditions at 300 °C. Characterization of fresh, reduced samples, by H2 chemisorption, TEM and FTIR spectroscopy of adsorbed of CO and NO, indicated that the promoter is not covering the metal surface. Under dry conditions the rate of N2 formation is lowered on the vanadia-modified alumina but the production of N2O was not altered. As a result the selectivity to N2 decreased markedly on Pd-VOx/γ-Al2O3. FTIR and XPS characterization of used catalysts demonstrated that the negative effect of VOx on N2 formation is due to an oxidized state of Pd that develops under reaction conditions. FTIR analysis of the gas phase products showed that both catalysts produce small amounts of gas phase HNCO and NH3 with the participation of surface -OH groups. FTIR spectra of the catalysts surface under reaction conditions demonstrate the presence of isocyanate (-NCO) and hydrogen containing compounds derived from HNCO. These stable species are not responsible for the production of N2O, but contribute to deactivation of the catalyst. They are rapidly eliminated upon water injection with a brief high production of NH3. Under steady state conditions water increases the CO conversion and the selectivity to N2 and NH3 on Pd/γ-Al2O3. The most notable effect is a marked reduction in N2O production. On Pd-VOx/γ-Al2O3 water increases the conversion of both NO and CO, as well as the NH3 formation. The selectivity to N2 is not altered and it is lower than the ones of NH3 and N2O. On both catalysts the NH3 formation increases due to the rapid hydrolysis of -NCO and HNCO. The H2 participation in the process of NH3 formation is excluded due to the very low activity of Pd/γ-Al2O3 and Pd-VOx/γ-Al2O3 for the water-gas shift reaction.
Fil: Neyertz, Claudia A.. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; Argentina
Fil: Volpe, María Alicia. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; Argentina
Fil: Perez, D.. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; Argentina
Fil: Costilla, Ignacio Oscar. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; Argentina
Fil: Sanchez, Miguel Dario. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; Argentina
Fil: Gigola, Carlos Eugenio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; Argentina
Materia
Ammonia Formation
Hnco
Isocyanate
Isocyanic Acid
No + Co
No + Co + H2o
Pd (Palladium)
V (Vanadium)
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:11336/62077
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/62077
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling NO reduction with CO in the presence and absence of H2O over Pd/γ-Al2O3 and Pd-VOx/γ-Al2O3 catalysts: The formation of HNCO, NH3 and stable surface speciesNeyertz, Claudia A.Volpe, María AliciaPerez, D.Costilla, Ignacio OscarSanchez, Miguel DarioGigola, Carlos EugenioAmmonia FormationHncoIsocyanateIsocyanic AcidNo + CoNo + Co + H2oPd (Palladium)V (Vanadium)https://purl.org/becyt/ford/2.4https://purl.org/becyt/ford/2The reduction of NO by CO over Pd/γ-Al2O3 and Pd-VOx/γ-Al2O3 catalysts has been studied by combining activity and selectivity measurements with FTIR spectroscopy of gas phase products and adsorbed species under reaction conditions at 300 °C. Characterization of fresh, reduced samples, by H2 chemisorption, TEM and FTIR spectroscopy of adsorbed of CO and NO, indicated that the promoter is not covering the metal surface. Under dry conditions the rate of N2 formation is lowered on the vanadia-modified alumina but the production of N2O was not altered. As a result the selectivity to N2 decreased markedly on Pd-VOx/γ-Al2O3. FTIR and XPS characterization of used catalysts demonstrated that the negative effect of VOx on N2 formation is due to an oxidized state of Pd that develops under reaction conditions. FTIR analysis of the gas phase products showed that both catalysts produce small amounts of gas phase HNCO and NH3 with the participation of surface -OH groups. FTIR spectra of the catalysts surface under reaction conditions demonstrate the presence of isocyanate (-NCO) and hydrogen containing compounds derived from HNCO. These stable species are not responsible for the production of N2O, but contribute to deactivation of the catalyst. They are rapidly eliminated upon water injection with a brief high production of NH3. Under steady state conditions water increases the CO conversion and the selectivity to N2 and NH3 on Pd/γ-Al2O3. The most notable effect is a marked reduction in N2O production. On Pd-VOx/γ-Al2O3 water increases the conversion of both NO and CO, as well as the NH3 formation. The selectivity to N2 is not altered and it is lower than the ones of NH3 and N2O. On both catalysts the NH3 formation increases due to the rapid hydrolysis of -NCO and HNCO. The H2 participation in the process of NH3 formation is excluded due to the very low activity of Pd/γ-Al2O3 and Pd-VOx/γ-Al2O3 for the water-gas shift reaction.Fil: Neyertz, Claudia A.. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; ArgentinaFil: Volpe, María Alicia. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; ArgentinaFil: Perez, D.. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; ArgentinaFil: Costilla, Ignacio Oscar. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; ArgentinaFil: Sanchez, Miguel Dario. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; ArgentinaFil: Gigola, Carlos Eugenio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; ArgentinaElsevier Science2009-10info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/62077Neyertz, Claudia A.; Volpe, María Alicia; Perez, D.; Costilla, Ignacio Oscar; Sanchez, Miguel Dario; et al.; NO reduction with CO in the presence and absence of H2O over Pd/γ-Al2O3 and Pd-VOx/γ-Al2O3 catalysts: The formation of HNCO, NH3 and stable surface species; Elsevier Science; Applied Catalysis A: General; 368; 1-2; 10-2009; 146-1570926-860XCONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1016/j.apcata.2009.08.023info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0926860X09005936info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-22T12:07:43Zoai:ri.conicet.gov.ar:11336/62077instacron: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:34982025-10-22 12:07:43.587CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv NO reduction with CO in the presence and absence of H2O over Pd/γ-Al2O3 and Pd-VOx/γ-Al2O3 catalysts: The formation of HNCO, NH3 and stable surface species
title NO reduction with CO in the presence and absence of H2O over Pd/γ-Al2O3 and Pd-VOx/γ-Al2O3 catalysts: The formation of HNCO, NH3 and stable surface species
spellingShingle NO reduction with CO in the presence and absence of H2O over Pd/γ-Al2O3 and Pd-VOx/γ-Al2O3 catalysts: The formation of HNCO, NH3 and stable surface species
Neyertz, Claudia A.
Ammonia Formation
Hnco
Isocyanate
Isocyanic Acid
No + Co
No + Co + H2o
Pd (Palladium)
V (Vanadium)
title_short NO reduction with CO in the presence and absence of H2O over Pd/γ-Al2O3 and Pd-VOx/γ-Al2O3 catalysts: The formation of HNCO, NH3 and stable surface species
title_full NO reduction with CO in the presence and absence of H2O over Pd/γ-Al2O3 and Pd-VOx/γ-Al2O3 catalysts: The formation of HNCO, NH3 and stable surface species
title_fullStr NO reduction with CO in the presence and absence of H2O over Pd/γ-Al2O3 and Pd-VOx/γ-Al2O3 catalysts: The formation of HNCO, NH3 and stable surface species
title_full_unstemmed NO reduction with CO in the presence and absence of H2O over Pd/γ-Al2O3 and Pd-VOx/γ-Al2O3 catalysts: The formation of HNCO, NH3 and stable surface species
title_sort NO reduction with CO in the presence and absence of H2O over Pd/γ-Al2O3 and Pd-VOx/γ-Al2O3 catalysts: The formation of HNCO, NH3 and stable surface species
dc.creator.none.fl_str_mv Neyertz, Claudia A.
Volpe, María Alicia
Perez, D.
Costilla, Ignacio Oscar
Sanchez, Miguel Dario
Gigola, Carlos Eugenio
author Neyertz, Claudia A.
author_facet Neyertz, Claudia A.
Volpe, María Alicia
Perez, D.
Costilla, Ignacio Oscar
Sanchez, Miguel Dario
Gigola, Carlos Eugenio
author_role author
author2 Volpe, María Alicia
Perez, D.
Costilla, Ignacio Oscar
Sanchez, Miguel Dario
Gigola, Carlos Eugenio
author2_role author
author
author
author
author
dc.subject.none.fl_str_mv Ammonia Formation
Hnco
Isocyanate
Isocyanic Acid
No + Co
No + Co + H2o
Pd (Palladium)
V (Vanadium)
topic Ammonia Formation
Hnco
Isocyanate
Isocyanic Acid
No + Co
No + Co + H2o
Pd (Palladium)
V (Vanadium)
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.4
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv The reduction of NO by CO over Pd/γ-Al2O3 and Pd-VOx/γ-Al2O3 catalysts has been studied by combining activity and selectivity measurements with FTIR spectroscopy of gas phase products and adsorbed species under reaction conditions at 300 °C. Characterization of fresh, reduced samples, by H2 chemisorption, TEM and FTIR spectroscopy of adsorbed of CO and NO, indicated that the promoter is not covering the metal surface. Under dry conditions the rate of N2 formation is lowered on the vanadia-modified alumina but the production of N2O was not altered. As a result the selectivity to N2 decreased markedly on Pd-VOx/γ-Al2O3. FTIR and XPS characterization of used catalysts demonstrated that the negative effect of VOx on N2 formation is due to an oxidized state of Pd that develops under reaction conditions. FTIR analysis of the gas phase products showed that both catalysts produce small amounts of gas phase HNCO and NH3 with the participation of surface -OH groups. FTIR spectra of the catalysts surface under reaction conditions demonstrate the presence of isocyanate (-NCO) and hydrogen containing compounds derived from HNCO. These stable species are not responsible for the production of N2O, but contribute to deactivation of the catalyst. They are rapidly eliminated upon water injection with a brief high production of NH3. Under steady state conditions water increases the CO conversion and the selectivity to N2 and NH3 on Pd/γ-Al2O3. The most notable effect is a marked reduction in N2O production. On Pd-VOx/γ-Al2O3 water increases the conversion of both NO and CO, as well as the NH3 formation. The selectivity to N2 is not altered and it is lower than the ones of NH3 and N2O. On both catalysts the NH3 formation increases due to the rapid hydrolysis of -NCO and HNCO. The H2 participation in the process of NH3 formation is excluded due to the very low activity of Pd/γ-Al2O3 and Pd-VOx/γ-Al2O3 for the water-gas shift reaction.
Fil: Neyertz, Claudia A.. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; Argentina
Fil: Volpe, María Alicia. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; Argentina
Fil: Perez, D.. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; Argentina
Fil: Costilla, Ignacio Oscar. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; Argentina
Fil: Sanchez, Miguel Dario. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; Argentina
Fil: Gigola, Carlos Eugenio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Bahía Blanca. Planta Piloto de Ingeniería Química. Universidad Nacional del Sur. Planta Piloto de Ingeniería Química; Argentina
description The reduction of NO by CO over Pd/γ-Al2O3 and Pd-VOx/γ-Al2O3 catalysts has been studied by combining activity and selectivity measurements with FTIR spectroscopy of gas phase products and adsorbed species under reaction conditions at 300 °C. Characterization of fresh, reduced samples, by H2 chemisorption, TEM and FTIR spectroscopy of adsorbed of CO and NO, indicated that the promoter is not covering the metal surface. Under dry conditions the rate of N2 formation is lowered on the vanadia-modified alumina but the production of N2O was not altered. As a result the selectivity to N2 decreased markedly on Pd-VOx/γ-Al2O3. FTIR and XPS characterization of used catalysts demonstrated that the negative effect of VOx on N2 formation is due to an oxidized state of Pd that develops under reaction conditions. FTIR analysis of the gas phase products showed that both catalysts produce small amounts of gas phase HNCO and NH3 with the participation of surface -OH groups. FTIR spectra of the catalysts surface under reaction conditions demonstrate the presence of isocyanate (-NCO) and hydrogen containing compounds derived from HNCO. These stable species are not responsible for the production of N2O, but contribute to deactivation of the catalyst. They are rapidly eliminated upon water injection with a brief high production of NH3. Under steady state conditions water increases the CO conversion and the selectivity to N2 and NH3 on Pd/γ-Al2O3. The most notable effect is a marked reduction in N2O production. On Pd-VOx/γ-Al2O3 water increases the conversion of both NO and CO, as well as the NH3 formation. The selectivity to N2 is not altered and it is lower than the ones of NH3 and N2O. On both catalysts the NH3 formation increases due to the rapid hydrolysis of -NCO and HNCO. The H2 participation in the process of NH3 formation is excluded due to the very low activity of Pd/γ-Al2O3 and Pd-VOx/γ-Al2O3 for the water-gas shift reaction.
publishDate 2009
dc.date.none.fl_str_mv 2009-10
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/11336/62077
Neyertz, Claudia A.; Volpe, María Alicia; Perez, D.; Costilla, Ignacio Oscar; Sanchez, Miguel Dario; et al.; NO reduction with CO in the presence and absence of H2O over Pd/γ-Al2O3 and Pd-VOx/γ-Al2O3 catalysts: The formation of HNCO, NH3 and stable surface species; Elsevier Science; Applied Catalysis A: General; 368; 1-2; 10-2009; 146-157
0926-860X
CONICET Digital
CONICET
url http://hdl.handle.net/11336/62077
identifier_str_mv Neyertz, Claudia A.; Volpe, María Alicia; Perez, D.; Costilla, Ignacio Oscar; Sanchez, Miguel Dario; et al.; NO reduction with CO in the presence and absence of H2O over Pd/γ-Al2O3 and Pd-VOx/γ-Al2O3 catalysts: The formation of HNCO, NH3 and stable surface species; Elsevier Science; Applied Catalysis A: General; 368; 1-2; 10-2009; 146-157
0926-860X
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1016/j.apcata.2009.08.023
info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0926860X09005936
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
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 12.982451

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