The SCR of NO with CH4 over Co-, Co,Pt-, and H-mordenite catalysts

Autores
Lónyi, F.; Valyon, J.; Gutierrez, Laura Beatriz; Ulla, Maria Alicia del H.; Lombardo, Eduardo Agustin
Año de publicación
2007
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The catalytic reduction of NO with methane was studied operando in the presence and absence of oxygen in the reaction mixture over Co-, Co,Pt-, and H-mordenite (CoM, CoPtM, HM) catalysts using the coupled methods of diffuse reflectance infrared Fourier-transform spectroscopy and mass spectroscopy (Operando-DRIFTS-MS). The reaction temperature was in the 573-773 K range, and the GHSV for nitric oxide was varied between 6000 and 60,000 h-1. In general, the Co-containing mordenite catalysts were more active than the HM. Over each catalyst two major surface intermediates were identified such as nitrosonium ion (NO+) and ammonia. The NO+ cations were shown to balance the negative charge on the zeolite framework. The NH3 molecules were bound either coordinately to Lewis-acid site Co2+ ions or were protonated on Brønsted acid sites and retained by the zeolite as NH4 + cations. The prevailing route of N2 formation was found to involve the reaction of NO+ and NH3 or NH4 + surface species. It was shown that the surface concentration of the intermediate ammonia governed the rate of NO conversion. If O2 was present in the feed gas it competed with the NO in the oxidation of methane and the surface intermediate ammonia. As a result, the steady-state concentration of the ammonia intermediate and the overall NO conversion to N2 decreased. Additional routes of N2 formation were revealed over the CoM and CoPtM catalysts. The cobalt facilitated the formation of NO+ and surface nitrate (NO3 -). Also nitrile (CN) and isocyanate (NCO) surface species were detected. The NO3 - could be rapidly reduced by methane to intermediate NH3 and, thereby, it increased the rate of NO conversion significantly. Nitrogen forming reactions can pass also through CN and NCO intermediates; however, the share of these reaction routes in the overall N2 generation process was minor.
Fil: Lónyi, F.. Chemical Research Center, Budapest;
Fil: Valyon, J.. Chemical Research Center, Budapest;
Fil: Gutierrez, Laura Beatriz. 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: Ulla, Maria Alicia del H.. 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: Lombardo, Eduardo Agustin. 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
Nox Abatement;
Co,Pt-Mordenite
Operando Drifts-Ms;
Ch4/No-Scr
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:11336/65323
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/65323
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling The SCR of NO with CH4 over Co-, Co,Pt-, and H-mordenite catalystsLónyi, F.Valyon, J.Gutierrez, Laura BeatrizUlla, Maria Alicia del H.Lombardo, Eduardo AgustinNox Abatement;Co,Pt-MordeniteOperando Drifts-Ms;Ch4/No-Scrhttps://purl.org/becyt/ford/2.4https://purl.org/becyt/ford/2The catalytic reduction of NO with methane was studied operando in the presence and absence of oxygen in the reaction mixture over Co-, Co,Pt-, and H-mordenite (CoM, CoPtM, HM) catalysts using the coupled methods of diffuse reflectance infrared Fourier-transform spectroscopy and mass spectroscopy (Operando-DRIFTS-MS). The reaction temperature was in the 573-773 K range, and the GHSV for nitric oxide was varied between 6000 and 60,000 h-1. In general, the Co-containing mordenite catalysts were more active than the HM. Over each catalyst two major surface intermediates were identified such as nitrosonium ion (NO+) and ammonia. The NO+ cations were shown to balance the negative charge on the zeolite framework. The NH3 molecules were bound either coordinately to Lewis-acid site Co2+ ions or were protonated on Brønsted acid sites and retained by the zeolite as NH4 + cations. The prevailing route of N2 formation was found to involve the reaction of NO+ and NH3 or NH4 + surface species. It was shown that the surface concentration of the intermediate ammonia governed the rate of NO conversion. If O2 was present in the feed gas it competed with the NO in the oxidation of methane and the surface intermediate ammonia. As a result, the steady-state concentration of the ammonia intermediate and the overall NO conversion to N2 decreased. Additional routes of N2 formation were revealed over the CoM and CoPtM catalysts. The cobalt facilitated the formation of NO+ and surface nitrate (NO3 -). Also nitrile (CN) and isocyanate (NCO) surface species were detected. The NO3 - could be rapidly reduced by methane to intermediate NH3 and, thereby, it increased the rate of NO conversion significantly. Nitrogen forming reactions can pass also through CN and NCO intermediates; however, the share of these reaction routes in the overall N2 generation process was minor.Fil: Lónyi, F.. Chemical Research Center, Budapest;Fil: Valyon, J.. Chemical Research Center, Budapest;Fil: Gutierrez, Laura Beatriz. 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: Ulla, Maria Alicia del H.. 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: Lombardo, Eduardo Agustin. 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 Science2007-04info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/65323Lónyi, F.; Valyon, J.; Gutierrez, Laura Beatriz; Ulla, Maria Alicia del H.; Lombardo, Eduardo Agustin; The SCR of NO with CH4 over Co-, Co,Pt-, and H-mordenite catalysts; Elsevier Science; Applied Catalysis B: Environmental; 73; 1-2; 4-2007; 1-100926-3373CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1016/j.apcatb.2006.11.017info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T09:44:37Zoai:ri.conicet.gov.ar:11336/65323instacron: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:34982025-09-03 09:44:37.272CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv The SCR of NO with CH4 over Co-, Co,Pt-, and H-mordenite catalysts
title The SCR of NO with CH4 over Co-, Co,Pt-, and H-mordenite catalysts
spellingShingle The SCR of NO with CH4 over Co-, Co,Pt-, and H-mordenite catalysts
Lónyi, F.
Nox Abatement;
Co,Pt-Mordenite
Operando Drifts-Ms;
Ch4/No-Scr
title_short The SCR of NO with CH4 over Co-, Co,Pt-, and H-mordenite catalysts
title_full The SCR of NO with CH4 over Co-, Co,Pt-, and H-mordenite catalysts
title_fullStr The SCR of NO with CH4 over Co-, Co,Pt-, and H-mordenite catalysts
title_full_unstemmed The SCR of NO with CH4 over Co-, Co,Pt-, and H-mordenite catalysts
title_sort The SCR of NO with CH4 over Co-, Co,Pt-, and H-mordenite catalysts
dc.creator.none.fl_str_mv Lónyi, F.
Valyon, J.
Gutierrez, Laura Beatriz
Ulla, Maria Alicia del H.
Lombardo, Eduardo Agustin
author Lónyi, F.
author_facet Lónyi, F.
Valyon, J.
Gutierrez, Laura Beatriz
Ulla, Maria Alicia del H.
Lombardo, Eduardo Agustin
author_role author
author2 Valyon, J.
Gutierrez, Laura Beatriz
Ulla, Maria Alicia del H.
Lombardo, Eduardo Agustin
author2_role author
author
author
author
dc.subject.none.fl_str_mv Nox Abatement;
Co,Pt-Mordenite
Operando Drifts-Ms;
Ch4/No-Scr
topic Nox Abatement;
Co,Pt-Mordenite
Operando Drifts-Ms;
Ch4/No-Scr
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 catalytic reduction of NO with methane was studied operando in the presence and absence of oxygen in the reaction mixture over Co-, Co,Pt-, and H-mordenite (CoM, CoPtM, HM) catalysts using the coupled methods of diffuse reflectance infrared Fourier-transform spectroscopy and mass spectroscopy (Operando-DRIFTS-MS). The reaction temperature was in the 573-773 K range, and the GHSV for nitric oxide was varied between 6000 and 60,000 h-1. In general, the Co-containing mordenite catalysts were more active than the HM. Over each catalyst two major surface intermediates were identified such as nitrosonium ion (NO+) and ammonia. The NO+ cations were shown to balance the negative charge on the zeolite framework. The NH3 molecules were bound either coordinately to Lewis-acid site Co2+ ions or were protonated on Brønsted acid sites and retained by the zeolite as NH4 + cations. The prevailing route of N2 formation was found to involve the reaction of NO+ and NH3 or NH4 + surface species. It was shown that the surface concentration of the intermediate ammonia governed the rate of NO conversion. If O2 was present in the feed gas it competed with the NO in the oxidation of methane and the surface intermediate ammonia. As a result, the steady-state concentration of the ammonia intermediate and the overall NO conversion to N2 decreased. Additional routes of N2 formation were revealed over the CoM and CoPtM catalysts. The cobalt facilitated the formation of NO+ and surface nitrate (NO3 -). Also nitrile (CN) and isocyanate (NCO) surface species were detected. The NO3 - could be rapidly reduced by methane to intermediate NH3 and, thereby, it increased the rate of NO conversion significantly. Nitrogen forming reactions can pass also through CN and NCO intermediates; however, the share of these reaction routes in the overall N2 generation process was minor.
Fil: Lónyi, F.. Chemical Research Center, Budapest;
Fil: Valyon, J.. Chemical Research Center, Budapest;
Fil: Gutierrez, Laura Beatriz. 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: Ulla, Maria Alicia del H.. 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: Lombardo, Eduardo Agustin. 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 The catalytic reduction of NO with methane was studied operando in the presence and absence of oxygen in the reaction mixture over Co-, Co,Pt-, and H-mordenite (CoM, CoPtM, HM) catalysts using the coupled methods of diffuse reflectance infrared Fourier-transform spectroscopy and mass spectroscopy (Operando-DRIFTS-MS). The reaction temperature was in the 573-773 K range, and the GHSV for nitric oxide was varied between 6000 and 60,000 h-1. In general, the Co-containing mordenite catalysts were more active than the HM. Over each catalyst two major surface intermediates were identified such as nitrosonium ion (NO+) and ammonia. The NO+ cations were shown to balance the negative charge on the zeolite framework. The NH3 molecules were bound either coordinately to Lewis-acid site Co2+ ions or were protonated on Brønsted acid sites and retained by the zeolite as NH4 + cations. The prevailing route of N2 formation was found to involve the reaction of NO+ and NH3 or NH4 + surface species. It was shown that the surface concentration of the intermediate ammonia governed the rate of NO conversion. If O2 was present in the feed gas it competed with the NO in the oxidation of methane and the surface intermediate ammonia. As a result, the steady-state concentration of the ammonia intermediate and the overall NO conversion to N2 decreased. Additional routes of N2 formation were revealed over the CoM and CoPtM catalysts. The cobalt facilitated the formation of NO+ and surface nitrate (NO3 -). Also nitrile (CN) and isocyanate (NCO) surface species were detected. The NO3 - could be rapidly reduced by methane to intermediate NH3 and, thereby, it increased the rate of NO conversion significantly. Nitrogen forming reactions can pass also through CN and NCO intermediates; however, the share of these reaction routes in the overall N2 generation process was minor.
publishDate 2007
dc.date.none.fl_str_mv 2007-04
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/11336/65323
Lónyi, F.; Valyon, J.; Gutierrez, Laura Beatriz; Ulla, Maria Alicia del H.; Lombardo, Eduardo Agustin; The SCR of NO with CH4 over Co-, Co,Pt-, and H-mordenite catalysts; Elsevier Science; Applied Catalysis B: Environmental; 73; 1-2; 4-2007; 1-10
0926-3373
CONICET Digital
CONICET
url http://hdl.handle.net/11336/65323
identifier_str_mv Lónyi, F.; Valyon, J.; Gutierrez, Laura Beatriz; Ulla, Maria Alicia del H.; Lombardo, Eduardo Agustin; The SCR of NO with CH4 over Co-, Co,Pt-, and H-mordenite catalysts; Elsevier Science; Applied Catalysis B: Environmental; 73; 1-2; 4-2007; 1-10
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.2006.11.017
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
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 13.13397

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