An operando DRIFTS study of the active sites and the active intermediates of the NO-SCR reaction by methane over In,H- and In,Pd,H-zeolite catalysts

Autores
Lónyi, Ferenc; Solt, Hanna E.; Valyon, József; Decolatti, Hernán Pablo; Gutierrez, Laura Beatriz; Miro, Eduardo Ernesto
Año de publicación
2010
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Zeolites In,H-ZSM-5 (Si/Al=29.7, 1.7wt% In) and In,H-mordenite (In,H-M, Si/Al=6.7, 3.5 wt% In) were prepared by reductive solid state ion exchange (RSSIE) method and studied in the selective catalytic reduction of NO (NO-SCR) by methane. The results suggested that the methane oxidation reactions proceed by redox type mechanisms over In+/InO+ sites. The NO reduction selectivity was shown to be related to the relative rates of In+ oxidation by NO and O2. Regarding the relative rates, the In+ density of the zeolite was the most important. Above about 673K the In,H-ZSM-5 (T-atom/In=102) had higher NO reduction selectivity than the In,H-mordenite (T-atom/In=46). The operando DRIFTS examinations suggested that NO+ and NO3 - surface species were formed simultaneously on InO+Z- sites, and were consumed together in the NO-SCR reaction with methane. The reduction of the NO3 - by methane gave an activated N-containing intermediate, which further reacted with the NO+ species to give N2. The NO-SCR properties could be significantly improved by adding small amount of Pd to the In,H-zeolite catalyst. The promoting effect of Pd was interpreted as a concerted action of InO+ and the Pdn+ sites. The interplay between these sites is twofold: the Pd speeds up the equilibration of the NO/O2 mixture, thereby, increases the formation rate and the steady state concentration of the activated nitrate species, whereas the In+/InO+ sites prevent the transformation of Pd-nitrosyls to less reactive isocyanate and nitrile species.
Fil: Lónyi, Ferenc. Chemical Research Center; Hungría
Fil: Solt, Hanna E.. Chemical Research Center; Hungría
Fil: Valyon, József. Chemical Research Center; Hungría
Fil: Decolatti, Hernán Pablo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Fil: Gutierrez, Laura Beatriz. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Fil: Miro, Eduardo Ernesto. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Materia
In,H-Zeolites
In,Pd,H-Zeolites
No-Scr by Ch4 Operando-Drifts
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:11336/54028
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/54028
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling An operando DRIFTS study of the active sites and the active intermediates of the NO-SCR reaction by methane over In,H- and In,Pd,H-zeolite catalystsLónyi, FerencSolt, Hanna E.Valyon, JózsefDecolatti, Hernán PabloGutierrez, Laura BeatrizMiro, Eduardo ErnestoIn,H-ZeolitesIn,Pd,H-ZeolitesNo-Scr by Ch4 Operando-Driftshttps://purl.org/becyt/ford/2.4https://purl.org/becyt/ford/2Zeolites In,H-ZSM-5 (Si/Al=29.7, 1.7wt% In) and In,H-mordenite (In,H-M, Si/Al=6.7, 3.5 wt% In) were prepared by reductive solid state ion exchange (RSSIE) method and studied in the selective catalytic reduction of NO (NO-SCR) by methane. The results suggested that the methane oxidation reactions proceed by redox type mechanisms over In+/InO+ sites. The NO reduction selectivity was shown to be related to the relative rates of In+ oxidation by NO and O2. Regarding the relative rates, the In+ density of the zeolite was the most important. Above about 673K the In,H-ZSM-5 (T-atom/In=102) had higher NO reduction selectivity than the In,H-mordenite (T-atom/In=46). The operando DRIFTS examinations suggested that NO+ and NO3 - surface species were formed simultaneously on InO+Z- sites, and were consumed together in the NO-SCR reaction with methane. The reduction of the NO3 - by methane gave an activated N-containing intermediate, which further reacted with the NO+ species to give N2. The NO-SCR properties could be significantly improved by adding small amount of Pd to the In,H-zeolite catalyst. The promoting effect of Pd was interpreted as a concerted action of InO+ and the Pdn+ sites. The interplay between these sites is twofold: the Pd speeds up the equilibration of the NO/O2 mixture, thereby, increases the formation rate and the steady state concentration of the activated nitrate species, whereas the In+/InO+ sites prevent the transformation of Pd-nitrosyls to less reactive isocyanate and nitrile species.Fil: Lónyi, Ferenc. Chemical Research Center; HungríaFil: Solt, Hanna E.. Chemical Research Center; HungríaFil: Valyon, József. Chemical Research Center; HungríaFil: Decolatti, Hernán Pablo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; ArgentinaFil: Gutierrez, Laura Beatriz. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; ArgentinaFil: Miro, Eduardo Ernesto. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; ArgentinaElsevier Science2010-07info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/54028Lónyi, Ferenc; Solt, Hanna E.; Valyon, József; Decolatti, Hernán Pablo; Gutierrez, Laura Beatriz; et al.; An operando DRIFTS study of the active sites and the active intermediates of the NO-SCR reaction by methane over In,H- and In,Pd,H-zeolite catalysts; Elsevier Science; Applied Catalysis B: Environmental; 100; 7-2010; 133-1420926-3373CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1016/j.apcatb.2010.07.023info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-15T14:24:02Zoai:ri.conicet.gov.ar:11336/54028instacron: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:34982025-10-15 14:24:03.11CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv An operando DRIFTS study of the active sites and the active intermediates of the NO-SCR reaction by methane over In,H- and In,Pd,H-zeolite catalysts
title An operando DRIFTS study of the active sites and the active intermediates of the NO-SCR reaction by methane over In,H- and In,Pd,H-zeolite catalysts
spellingShingle An operando DRIFTS study of the active sites and the active intermediates of the NO-SCR reaction by methane over In,H- and In,Pd,H-zeolite catalysts
Lónyi, Ferenc
In,H-Zeolites
In,Pd,H-Zeolites
No-Scr by Ch4 Operando-Drifts
title_short An operando DRIFTS study of the active sites and the active intermediates of the NO-SCR reaction by methane over In,H- and In,Pd,H-zeolite catalysts
title_full An operando DRIFTS study of the active sites and the active intermediates of the NO-SCR reaction by methane over In,H- and In,Pd,H-zeolite catalysts
title_fullStr An operando DRIFTS study of the active sites and the active intermediates of the NO-SCR reaction by methane over In,H- and In,Pd,H-zeolite catalysts
title_full_unstemmed An operando DRIFTS study of the active sites and the active intermediates of the NO-SCR reaction by methane over In,H- and In,Pd,H-zeolite catalysts
title_sort An operando DRIFTS study of the active sites and the active intermediates of the NO-SCR reaction by methane over In,H- and In,Pd,H-zeolite catalysts
dc.creator.none.fl_str_mv Lónyi, Ferenc
Solt, Hanna E.
Valyon, József
Decolatti, Hernán Pablo
Gutierrez, Laura Beatriz
Miro, Eduardo Ernesto
author Lónyi, Ferenc
author_facet Lónyi, Ferenc
Solt, Hanna E.
Valyon, József
Decolatti, Hernán Pablo
Gutierrez, Laura Beatriz
Miro, Eduardo Ernesto
author_role author
author2 Solt, Hanna E.
Valyon, József
Decolatti, Hernán Pablo
Gutierrez, Laura Beatriz
Miro, Eduardo Ernesto
author2_role author
author
author
author
author
dc.subject.none.fl_str_mv In,H-Zeolites
In,Pd,H-Zeolites
No-Scr by Ch4 Operando-Drifts
topic In,H-Zeolites
In,Pd,H-Zeolites
No-Scr by Ch4 Operando-Drifts
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.4
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv Zeolites In,H-ZSM-5 (Si/Al=29.7, 1.7wt% In) and In,H-mordenite (In,H-M, Si/Al=6.7, 3.5 wt% In) were prepared by reductive solid state ion exchange (RSSIE) method and studied in the selective catalytic reduction of NO (NO-SCR) by methane. The results suggested that the methane oxidation reactions proceed by redox type mechanisms over In+/InO+ sites. The NO reduction selectivity was shown to be related to the relative rates of In+ oxidation by NO and O2. Regarding the relative rates, the In+ density of the zeolite was the most important. Above about 673K the In,H-ZSM-5 (T-atom/In=102) had higher NO reduction selectivity than the In,H-mordenite (T-atom/In=46). The operando DRIFTS examinations suggested that NO+ and NO3 - surface species were formed simultaneously on InO+Z- sites, and were consumed together in the NO-SCR reaction with methane. The reduction of the NO3 - by methane gave an activated N-containing intermediate, which further reacted with the NO+ species to give N2. The NO-SCR properties could be significantly improved by adding small amount of Pd to the In,H-zeolite catalyst. The promoting effect of Pd was interpreted as a concerted action of InO+ and the Pdn+ sites. The interplay between these sites is twofold: the Pd speeds up the equilibration of the NO/O2 mixture, thereby, increases the formation rate and the steady state concentration of the activated nitrate species, whereas the In+/InO+ sites prevent the transformation of Pd-nitrosyls to less reactive isocyanate and nitrile species.
Fil: Lónyi, Ferenc. Chemical Research Center; Hungría
Fil: Solt, Hanna E.. Chemical Research Center; Hungría
Fil: Valyon, József. Chemical Research Center; Hungría
Fil: Decolatti, Hernán Pablo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Fil: Gutierrez, Laura Beatriz. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
Fil: Miro, Eduardo Ernesto. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones en Catálisis y Petroquímica ; Argentina
description Zeolites In,H-ZSM-5 (Si/Al=29.7, 1.7wt% In) and In,H-mordenite (In,H-M, Si/Al=6.7, 3.5 wt% In) were prepared by reductive solid state ion exchange (RSSIE) method and studied in the selective catalytic reduction of NO (NO-SCR) by methane. The results suggested that the methane oxidation reactions proceed by redox type mechanisms over In+/InO+ sites. The NO reduction selectivity was shown to be related to the relative rates of In+ oxidation by NO and O2. Regarding the relative rates, the In+ density of the zeolite was the most important. Above about 673K the In,H-ZSM-5 (T-atom/In=102) had higher NO reduction selectivity than the In,H-mordenite (T-atom/In=46). The operando DRIFTS examinations suggested that NO+ and NO3 - surface species were formed simultaneously on InO+Z- sites, and were consumed together in the NO-SCR reaction with methane. The reduction of the NO3 - by methane gave an activated N-containing intermediate, which further reacted with the NO+ species to give N2. The NO-SCR properties could be significantly improved by adding small amount of Pd to the In,H-zeolite catalyst. The promoting effect of Pd was interpreted as a concerted action of InO+ and the Pdn+ sites. The interplay between these sites is twofold: the Pd speeds up the equilibration of the NO/O2 mixture, thereby, increases the formation rate and the steady state concentration of the activated nitrate species, whereas the In+/InO+ sites prevent the transformation of Pd-nitrosyls to less reactive isocyanate and nitrile species.
publishDate 2010
dc.date.none.fl_str_mv 2010-07
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/11336/54028
Lónyi, Ferenc; Solt, Hanna E.; Valyon, József; Decolatti, Hernán Pablo; Gutierrez, Laura Beatriz; et al.; An operando DRIFTS study of the active sites and the active intermediates of the NO-SCR reaction by methane over In,H- and In,Pd,H-zeolite catalysts; Elsevier Science; Applied Catalysis B: Environmental; 100; 7-2010; 133-142
0926-3373
CONICET Digital
CONICET
url http://hdl.handle.net/11336/54028
identifier_str_mv Lónyi, Ferenc; Solt, Hanna E.; Valyon, József; Decolatti, Hernán Pablo; Gutierrez, Laura Beatriz; et al.; An operando DRIFTS study of the active sites and the active intermediates of the NO-SCR reaction by methane over In,H- and In,Pd,H-zeolite catalysts; Elsevier Science; Applied Catalysis B: Environmental; 100; 7-2010; 133-142
0926-3373
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.apcatb.2010.07.023
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 13.22299

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