Evolution of Copper Nanospecies in the Synthesis Stages of MCM-41-Type Mesoporous Molecular Sieves

Autores
Chanquia, Corina Mercedes; Winkler, Elin Lilian; Causa, María T.; Eimer, Griselda Alejandra
Año de publicación
2012
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The redox behavior of copper nanospecies in the synthesis stages of MCM-41-type materials has been followed by ESR technique. These coppermodified mesoporous molecular sieves (Cu-MMS) were synthesized by direct incorporation method, and different treatments of the initial synthesis gel were evaluated. From ESR and UVVis-DRS data, a synergistic approach about the distribution of copper species in the different catalysts has been made: the hydrothermal treatment favors the incorporation of isolated cooper species into the framework, whereas both the aging treatment and the lack of subsequent treatment promote the formation of copper clusters into the mesoporous channels. The Hamiltonian parameters g// = 2.3 and g = 2.06 have confirmed the presence of isolated Cu2+ ions in octahedral coordination with tetragonal distortion within siliceous framework, whereas the g = 2.2 value was assigned to the presence of Cu2+ clusters. Only the catalyst aged at room temperature has presented additional signals characteristic of Cu2+ dimers. Finally, it is found that during the template removal process at 773 K the so-called self-reduction phenomenon of isolated cupric ions takes place: a 50-70% decrease in the ESR signal intensity was observed for the final Cu-MMS.
Fil: Chanquia, Corina Mercedes. Universidad Tecnológica Nacional. Facultad Regional Córdoba; Argentina. Comisión Nacional de Energía Atómica. Centro Atómico Bariloche; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; Argentina
Fil: Winkler, Elin Lilian. Comisión Nacional de Energía Atómica. Gerencia del Área de Investigación y Aplicaciones No Nucleares. Gerencia de Física (Centro Atómico Bariloche); Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; Argentina
Fil: Causa, María T.. Comisión Nacional de Energía Atómica. Gerencia del Área de Investigación y Aplicaciones No Nucleares. Gerencia de Física (Centro Atómico Bariloche); Argentina
Fil: Eimer, Griselda Alejandra. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; Argentina. Comisión Nacional de Energía Atómica. Centro Atómico Bariloche; Argentina. Universidad Tecnológica Nacional. Facultad Regional Córdoba; Argentina
Materia
COPPER
NANO-SPECIES
OXIDATION STATE
ESR
MCM-41
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:11336/268403
Acceder
id CONICETDig_5570b0b32d09c2ca51cc1433a49f086e
oai_identifier_str oai:ri.conicet.gov.ar:11336/268403
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Evolution of Copper Nanospecies in the Synthesis Stages of MCM-41-Type Mesoporous Molecular SievesChanquia, Corina MercedesWinkler, Elin LilianCausa, María T.Eimer, Griselda AlejandraCOPPERNANO-SPECIESOXIDATION STATEESRMCM-41https://purl.org/becyt/ford/2.10https://purl.org/becyt/ford/2The redox behavior of copper nanospecies in the synthesis stages of MCM-41-type materials has been followed by ESR technique. These coppermodified mesoporous molecular sieves (Cu-MMS) were synthesized by direct incorporation method, and different treatments of the initial synthesis gel were evaluated. From ESR and UVVis-DRS data, a synergistic approach about the distribution of copper species in the different catalysts has been made: the hydrothermal treatment favors the incorporation of isolated cooper species into the framework, whereas both the aging treatment and the lack of subsequent treatment promote the formation of copper clusters into the mesoporous channels. The Hamiltonian parameters g// = 2.3 and g = 2.06 have confirmed the presence of isolated Cu2+ ions in octahedral coordination with tetragonal distortion within siliceous framework, whereas the g = 2.2 value was assigned to the presence of Cu2+ clusters. Only the catalyst aged at room temperature has presented additional signals characteristic of Cu2+ dimers. Finally, it is found that during the template removal process at 773 K the so-called self-reduction phenomenon of isolated cupric ions takes place: a 50-70% decrease in the ESR signal intensity was observed for the final Cu-MMS.Fil: Chanquia, Corina Mercedes. Universidad Tecnológica Nacional. Facultad Regional Córdoba; Argentina. Comisión Nacional de Energía Atómica. Centro Atómico Bariloche; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; ArgentinaFil: Winkler, Elin Lilian. Comisión Nacional de Energía Atómica. Gerencia del Área de Investigación y Aplicaciones No Nucleares. Gerencia de Física (Centro Atómico Bariloche); Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; ArgentinaFil: Causa, María T.. Comisión Nacional de Energía Atómica. Gerencia del Área de Investigación y Aplicaciones No Nucleares. Gerencia de Física (Centro Atómico Bariloche); ArgentinaFil: Eimer, Griselda Alejandra. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; Argentina. Comisión Nacional de Energía Atómica. Centro Atómico Bariloche; Argentina. Universidad Tecnológica Nacional. Facultad Regional Córdoba; ArgentinaAmerican Chemical Society2012-02info: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/11336/268403Chanquia, Corina Mercedes; Winkler, Elin Lilian; Causa, María T.; Eimer, Griselda Alejandra; Evolution of Copper Nanospecies in the Synthesis Stages of MCM-41-Type Mesoporous Molecular Sieves; American Chemical Society; Journal of Physical Chemistry C; 116; 9; 2-2012; 5376-53821932-7447CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/abs/10.1021/jp210652xinfo:eu-repo/semantics/altIdentifier/doi/10.1021/jp210652xinfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T10:00:36Zoai:ri.conicet.gov.ar:11336/268403instacron: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 10:00:36.982CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Evolution of Copper Nanospecies in the Synthesis Stages of MCM-41-Type Mesoporous Molecular Sieves
title Evolution of Copper Nanospecies in the Synthesis Stages of MCM-41-Type Mesoporous Molecular Sieves
spellingShingle Evolution of Copper Nanospecies in the Synthesis Stages of MCM-41-Type Mesoporous Molecular Sieves
Chanquia, Corina Mercedes
COPPER
NANO-SPECIES
OXIDATION STATE
ESR
MCM-41
title_short Evolution of Copper Nanospecies in the Synthesis Stages of MCM-41-Type Mesoporous Molecular Sieves
title_full Evolution of Copper Nanospecies in the Synthesis Stages of MCM-41-Type Mesoporous Molecular Sieves
title_fullStr Evolution of Copper Nanospecies in the Synthesis Stages of MCM-41-Type Mesoporous Molecular Sieves
title_full_unstemmed Evolution of Copper Nanospecies in the Synthesis Stages of MCM-41-Type Mesoporous Molecular Sieves
title_sort Evolution of Copper Nanospecies in the Synthesis Stages of MCM-41-Type Mesoporous Molecular Sieves
dc.creator.none.fl_str_mv Chanquia, Corina Mercedes
Winkler, Elin Lilian
Causa, María T.
Eimer, Griselda Alejandra
author Chanquia, Corina Mercedes
author_facet Chanquia, Corina Mercedes
Winkler, Elin Lilian
Causa, María T.
Eimer, Griselda Alejandra
author_role author
author2 Winkler, Elin Lilian
Causa, María T.
Eimer, Griselda Alejandra
author2_role author
author
author
dc.subject.none.fl_str_mv COPPER
NANO-SPECIES
OXIDATION STATE
ESR
MCM-41
topic COPPER
NANO-SPECIES
OXIDATION STATE
ESR
MCM-41
purl_subject.fl_str_mv https://purl.org/becyt/ford/2.10
https://purl.org/becyt/ford/2
dc.description.none.fl_txt_mv The redox behavior of copper nanospecies in the synthesis stages of MCM-41-type materials has been followed by ESR technique. These coppermodified mesoporous molecular sieves (Cu-MMS) were synthesized by direct incorporation method, and different treatments of the initial synthesis gel were evaluated. From ESR and UVVis-DRS data, a synergistic approach about the distribution of copper species in the different catalysts has been made: the hydrothermal treatment favors the incorporation of isolated cooper species into the framework, whereas both the aging treatment and the lack of subsequent treatment promote the formation of copper clusters into the mesoporous channels. The Hamiltonian parameters g// = 2.3 and g = 2.06 have confirmed the presence of isolated Cu2+ ions in octahedral coordination with tetragonal distortion within siliceous framework, whereas the g = 2.2 value was assigned to the presence of Cu2+ clusters. Only the catalyst aged at room temperature has presented additional signals characteristic of Cu2+ dimers. Finally, it is found that during the template removal process at 773 K the so-called self-reduction phenomenon of isolated cupric ions takes place: a 50-70% decrease in the ESR signal intensity was observed for the final Cu-MMS.
Fil: Chanquia, Corina Mercedes. Universidad Tecnológica Nacional. Facultad Regional Córdoba; Argentina. Comisión Nacional de Energía Atómica. Centro Atómico Bariloche; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; Argentina
Fil: Winkler, Elin Lilian. Comisión Nacional de Energía Atómica. Gerencia del Área de Investigación y Aplicaciones No Nucleares. Gerencia de Física (Centro Atómico Bariloche); Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; Argentina
Fil: Causa, María T.. Comisión Nacional de Energía Atómica. Gerencia del Área de Investigación y Aplicaciones No Nucleares. Gerencia de Física (Centro Atómico Bariloche); Argentina
Fil: Eimer, Griselda Alejandra. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Patagonia Norte; Argentina. Comisión Nacional de Energía Atómica. Centro Atómico Bariloche; Argentina. Universidad Tecnológica Nacional. Facultad Regional Córdoba; Argentina
description The redox behavior of copper nanospecies in the synthesis stages of MCM-41-type materials has been followed by ESR technique. These coppermodified mesoporous molecular sieves (Cu-MMS) were synthesized by direct incorporation method, and different treatments of the initial synthesis gel were evaluated. From ESR and UVVis-DRS data, a synergistic approach about the distribution of copper species in the different catalysts has been made: the hydrothermal treatment favors the incorporation of isolated cooper species into the framework, whereas both the aging treatment and the lack of subsequent treatment promote the formation of copper clusters into the mesoporous channels. The Hamiltonian parameters g// = 2.3 and g = 2.06 have confirmed the presence of isolated Cu2+ ions in octahedral coordination with tetragonal distortion within siliceous framework, whereas the g = 2.2 value was assigned to the presence of Cu2+ clusters. Only the catalyst aged at room temperature has presented additional signals characteristic of Cu2+ dimers. Finally, it is found that during the template removal process at 773 K the so-called self-reduction phenomenon of isolated cupric ions takes place: a 50-70% decrease in the ESR signal intensity was observed for the final Cu-MMS.
publishDate 2012
dc.date.none.fl_str_mv 2012-02
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/11336/268403
Chanquia, Corina Mercedes; Winkler, Elin Lilian; Causa, María T.; Eimer, Griselda Alejandra; Evolution of Copper Nanospecies in the Synthesis Stages of MCM-41-Type Mesoporous Molecular Sieves; American Chemical Society; Journal of Physical Chemistry C; 116; 9; 2-2012; 5376-5382
1932-7447
CONICET Digital
CONICET
url http://hdl.handle.net/11336/268403
identifier_str_mv Chanquia, Corina Mercedes; Winkler, Elin Lilian; Causa, María T.; Eimer, Griselda Alejandra; Evolution of Copper Nanospecies in the Synthesis Stages of MCM-41-Type Mesoporous Molecular Sieves; American Chemical Society; Journal of Physical Chemistry C; 116; 9; 2-2012; 5376-5382
1932-7447
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/abs/10.1021/jp210652x
info:eu-repo/semantics/altIdentifier/doi/10.1021/jp210652x
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 American Chemical Society
publisher.none.fl_str_mv American Chemical Society
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_ 1842269648667541504
score 13.13397

Publicaciones similares