Gas phase imidazole methylation on zeolites and HPA/SiO2: Study of acid site requirements and catalyst deactivation

Autores
Vanoy Villamil, Michael Nicolás; Apesteguia, Carlos Rodolfo; Padro, Cristina
Año de publicación
2013
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The gas-phase alkylation of imidazole with methanol was studied at 523 K on solid acids such as HPA/SiO2 and zeolites HMCM22, HBEA, NaY, ZnY and HY. The nature, density and strength of acid sites were determined by temperature programmed desorption of NH3 coupled with infrared spectra of adsorbed pyridine. Coke formation was studied by temperature programmed oxidation technique. On all the samples, the selectivity to N-methylimidazole was greater than 98%. Catalysts presenting essentially Lewis (NaY and ZnY) or Brønsted (HPA/SiO2) acidity did not promote efficiently the methylation of imidazole and yielded less than 20% of N-methylimidazole. In contrast, on samples containing similar concentration of Lewis and Brønsted acid sites (HY, HBEA, HMCM22) the N-methylimidazole yield was between 60 % (HMCM22) and 100% (HY). All the samples deactivated during the 4 h catalytic tests and formed significant amounts of coke, between 2.3% (NaY) and 8% (ZnY). Catalytic tests performed at different contact times showed that the initial activity decay diminished with increasing imidazole conversion, suggesting that catalyst deactivation is mainly related with the presence of the reactants, methanol and/or imidazole. In order to gain insight on the catalyst deactivation mechanism, additional catalytic tests using different feed compositions were performed. They showed that the initial catalyst deactivation followed a linear correlation with the partial pressure of imidazole which indicated that the activity decay is essentially related with strong adsorption of imidazole the on surface acid sites.
Fil: Vanoy Villamil, Michael Nicolás. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera"; Argentina
Fil: Apesteguia, Carlos Rodolfo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera"; Argentina
Fil: Padro, Cristina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera"; Argentina
Materia
IMIDAZOLE METHYLATION
CATALYTS DEACTIVATION
SOLID ACIDS
DEACTIVATION MECHANISM
N-methylimidazole
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:11336/22421
Acceder
id CONICETDig_52795f0305b4bfa439ae96eba6cdd450
oai_identifier_str oai:ri.conicet.gov.ar:11336/22421
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Gas phase imidazole methylation on zeolites and HPA/SiO2: Study of acid site requirements and catalyst deactivationVanoy Villamil, Michael NicolásApesteguia, Carlos RodolfoPadro, CristinaIMIDAZOLE METHYLATIONCATALYTS DEACTIVATIONSOLID ACIDSDEACTIVATION MECHANISMN-methylimidazolehttps://purl.org/becyt/ford/2.4https://purl.org/becyt/ford/2The gas-phase alkylation of imidazole with methanol was studied at 523 K on solid acids such as HPA/SiO2 and zeolites HMCM22, HBEA, NaY, ZnY and HY. The nature, density and strength of acid sites were determined by temperature programmed desorption of NH3 coupled with infrared spectra of adsorbed pyridine. Coke formation was studied by temperature programmed oxidation technique. On all the samples, the selectivity to N-methylimidazole was greater than 98%. Catalysts presenting essentially Lewis (NaY and ZnY) or Brønsted (HPA/SiO2) acidity did not promote efficiently the methylation of imidazole and yielded less than 20% of N-methylimidazole. In contrast, on samples containing similar concentration of Lewis and Brønsted acid sites (HY, HBEA, HMCM22) the N-methylimidazole yield was between 60 % (HMCM22) and 100% (HY). All the samples deactivated during the 4 h catalytic tests and formed significant amounts of coke, between 2.3% (NaY) and 8% (ZnY). Catalytic tests performed at different contact times showed that the initial activity decay diminished with increasing imidazole conversion, suggesting that catalyst deactivation is mainly related with the presence of the reactants, methanol and/or imidazole. In order to gain insight on the catalyst deactivation mechanism, additional catalytic tests using different feed compositions were performed. They showed that the initial catalyst deactivation followed a linear correlation with the partial pressure of imidazole which indicated that the activity decay is essentially related with strong adsorption of imidazole the on surface acid sites.Fil: Vanoy Villamil, Michael Nicolás. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera"; ArgentinaFil: Apesteguia, Carlos Rodolfo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera"; ArgentinaFil: Padro, Cristina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera"; ArgentinaElsevier Inc2013-07info: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/11336/22421Vanoy Villamil, Michael Nicolás; Apesteguia, Carlos Rodolfo; Padro, Cristina; Gas phase imidazole methylation on zeolites and HPA/SiO2: Study of acid site requirements and catalyst deactivation; Elsevier Inc; Microporous and Mesoporous Materials; 181; 7-2013; 54-601387-1811CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1016/j.micromeso.2013.07.016info:eu-repo/semantics/altIdentifier/url/http://www.sciencedirect.com/science/article/pii/S1387181113003521info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-15T15:00:38Zoai:ri.conicet.gov.ar:11336/22421instacron: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 15:00:38.7CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Gas phase imidazole methylation on zeolites and HPA/SiO2: Study of acid site requirements and catalyst deactivation
title Gas phase imidazole methylation on zeolites and HPA/SiO2: Study of acid site requirements and catalyst deactivation
spellingShingle Gas phase imidazole methylation on zeolites and HPA/SiO2: Study of acid site requirements and catalyst deactivation
Vanoy Villamil, Michael Nicolás
IMIDAZOLE METHYLATION
CATALYTS DEACTIVATION
SOLID ACIDS
DEACTIVATION MECHANISM
N-methylimidazole
title_short Gas phase imidazole methylation on zeolites and HPA/SiO2: Study of acid site requirements and catalyst deactivation
title_full Gas phase imidazole methylation on zeolites and HPA/SiO2: Study of acid site requirements and catalyst deactivation
title_fullStr Gas phase imidazole methylation on zeolites and HPA/SiO2: Study of acid site requirements and catalyst deactivation
title_full_unstemmed Gas phase imidazole methylation on zeolites and HPA/SiO2: Study of acid site requirements and catalyst deactivation
title_sort Gas phase imidazole methylation on zeolites and HPA/SiO2: Study of acid site requirements and catalyst deactivation
dc.creator.none.fl_str_mv Vanoy Villamil, Michael Nicolás
Apesteguia, Carlos Rodolfo
Padro, Cristina
author Vanoy Villamil, Michael Nicolás
author_facet Vanoy Villamil, Michael Nicolás
Apesteguia, Carlos Rodolfo
Padro, Cristina
author_role author
author2 Apesteguia, Carlos Rodolfo
Padro, Cristina
author2_role author
author
dc.subject.none.fl_str_mv IMIDAZOLE METHYLATION
CATALYTS DEACTIVATION
SOLID ACIDS
DEACTIVATION MECHANISM
N-methylimidazole
topic IMIDAZOLE METHYLATION
CATALYTS DEACTIVATION
SOLID ACIDS
DEACTIVATION MECHANISM
N-methylimidazole
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 gas-phase alkylation of imidazole with methanol was studied at 523 K on solid acids such as HPA/SiO2 and zeolites HMCM22, HBEA, NaY, ZnY and HY. The nature, density and strength of acid sites were determined by temperature programmed desorption of NH3 coupled with infrared spectra of adsorbed pyridine. Coke formation was studied by temperature programmed oxidation technique. On all the samples, the selectivity to N-methylimidazole was greater than 98%. Catalysts presenting essentially Lewis (NaY and ZnY) or Brønsted (HPA/SiO2) acidity did not promote efficiently the methylation of imidazole and yielded less than 20% of N-methylimidazole. In contrast, on samples containing similar concentration of Lewis and Brønsted acid sites (HY, HBEA, HMCM22) the N-methylimidazole yield was between 60 % (HMCM22) and 100% (HY). All the samples deactivated during the 4 h catalytic tests and formed significant amounts of coke, between 2.3% (NaY) and 8% (ZnY). Catalytic tests performed at different contact times showed that the initial activity decay diminished with increasing imidazole conversion, suggesting that catalyst deactivation is mainly related with the presence of the reactants, methanol and/or imidazole. In order to gain insight on the catalyst deactivation mechanism, additional catalytic tests using different feed compositions were performed. They showed that the initial catalyst deactivation followed a linear correlation with the partial pressure of imidazole which indicated that the activity decay is essentially related with strong adsorption of imidazole the on surface acid sites.
Fil: Vanoy Villamil, Michael Nicolás. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera"; Argentina
Fil: Apesteguia, Carlos Rodolfo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera"; Argentina
Fil: Padro, Cristina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Santa Fe. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera". Universidad Nacional del Litoral. Instituto de Investigaciones En Catalisis y Petroquímica "ing. Jose Miguel Parera"; Argentina
description The gas-phase alkylation of imidazole with methanol was studied at 523 K on solid acids such as HPA/SiO2 and zeolites HMCM22, HBEA, NaY, ZnY and HY. The nature, density and strength of acid sites were determined by temperature programmed desorption of NH3 coupled with infrared spectra of adsorbed pyridine. Coke formation was studied by temperature programmed oxidation technique. On all the samples, the selectivity to N-methylimidazole was greater than 98%. Catalysts presenting essentially Lewis (NaY and ZnY) or Brønsted (HPA/SiO2) acidity did not promote efficiently the methylation of imidazole and yielded less than 20% of N-methylimidazole. In contrast, on samples containing similar concentration of Lewis and Brønsted acid sites (HY, HBEA, HMCM22) the N-methylimidazole yield was between 60 % (HMCM22) and 100% (HY). All the samples deactivated during the 4 h catalytic tests and formed significant amounts of coke, between 2.3% (NaY) and 8% (ZnY). Catalytic tests performed at different contact times showed that the initial activity decay diminished with increasing imidazole conversion, suggesting that catalyst deactivation is mainly related with the presence of the reactants, methanol and/or imidazole. In order to gain insight on the catalyst deactivation mechanism, additional catalytic tests using different feed compositions were performed. They showed that the initial catalyst deactivation followed a linear correlation with the partial pressure of imidazole which indicated that the activity decay is essentially related with strong adsorption of imidazole the on surface acid sites.
publishDate 2013
dc.date.none.fl_str_mv 2013-07
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/11336/22421
Vanoy Villamil, Michael Nicolás; Apesteguia, Carlos Rodolfo; Padro, Cristina; Gas phase imidazole methylation on zeolites and HPA/SiO2: Study of acid site requirements and catalyst deactivation; Elsevier Inc; Microporous and Mesoporous Materials; 181; 7-2013; 54-60
1387-1811
CONICET Digital
CONICET
url http://hdl.handle.net/11336/22421
identifier_str_mv Vanoy Villamil, Michael Nicolás; Apesteguia, Carlos Rodolfo; Padro, Cristina; Gas phase imidazole methylation on zeolites and HPA/SiO2: Study of acid site requirements and catalyst deactivation; Elsevier Inc; Microporous and Mesoporous Materials; 181; 7-2013; 54-60
1387-1811
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.micromeso.2013.07.016
info:eu-repo/semantics/altIdentifier/url/http://www.sciencedirect.com/science/article/pii/S1387181113003521
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 Inc
publisher.none.fl_str_mv Elsevier Inc
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
_version_ 1846083145755000832
score 13.22299

Publicaciones similares