XPS studies on the Cu(I,II)-polyampholyte heterogeneous catalyst: An insight into its structure and mechanism

Autores
Lazaro Martinez, Juan Manuel; Rodríguez Castellón, Enrique; Torres Sanchez, Rosa Maria; Denaday, Lisandro Roberto; Buldain, Graciela Yolanda; Campodallorto, Viviana
Año de publicación
2011
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
A complex between Cu(II) and a polyampholyte synthesized from methacrylic acid, imidazole and ethyleneglycol diglycidyl ether was used as a heterogeneous catalyst for hydrogen peroxide activation and degradation of chlorophenols. The material was characterized by XPS and by measurements of the zeta potential. The isoelectric point determined experimentally was 8.0, differing from that obtained by titration (6.4), which indicated the presence of fixed positive charges in disubstituted imidazole units. The XPS N 1s signal for pyridinic nitrogen in the imidazole units, and the O 1s signals from the carbonyl, hydroxyl and carboxylate groups shifted to higher binding energies after copper uptake, proving the chemical nature of Cu(II) adsorption on the polyampholyte. The XPS spectrum of the complex showed a Cu 2p3/2 peak at 934.7 eV and the characteristic shake-up satellite of Cu(II). When the complex was used as a heterogeneous catalyst for H2O2 activation, Cu(I) was proved to be a probable intermediate species and contributed to elucidate the mechanism. The Auger CuLMM spectrum supports the presence of Cu(I) with a kinetic energy value of 914.8 eV. The complex was applied in the oxidation of chlorinated phenols in aqueous solution at room temperature without any loss in efficiency. © 2011 Elsevier B.V. All rights reserved.
Fil: Lazaro Martinez, Juan Manuel. Universidad de Buenos Aires. Facultad de Farmacia y Bioquímica. Departamento de Química Orgánica; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Rodríguez Castellón, Enrique. Universidad de Málaga; España
Fil: Torres Sanchez, Rosa Maria. Provincia de Buenos Aires. Gobernación. Comisión de Investigaciones Científicas. Centro de Tecnología de Recursos Minerales y Cerámica. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Centro de Tecnología de Recursos Minerales y Cerámica; Argentina
Fil: Denaday, Lisandro Roberto. Universidad de Buenos Aires. Facultad de Farmacia y Bioquímica. Departamento de Química Analítica y Fisicoquímica; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Buldain, Graciela Yolanda. Universidad de Buenos Aires. Facultad de Farmacia y Bioquímica. Departamento de Química Orgánica; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Campodallorto, Viviana. Universidad de Buenos Aires. Facultad de Farmacia y Bioquímica. Departamento de Química Analítica y Fisicoquímica; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Materia
CHLORINATED PHENOLS
COPPER COMPLEX
HETEROGENEOUS CATALYST
POLYAMPHOLYTE
XPS
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:11336/151987
Acceder
id CONICETDig_d5c67c2fb3113aada8898a73ee4e9d84
oai_identifier_str oai:ri.conicet.gov.ar:11336/151987
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling XPS studies on the Cu(I,II)-polyampholyte heterogeneous catalyst: An insight into its structure and mechanismLazaro Martinez, Juan ManuelRodríguez Castellón, EnriqueTorres Sanchez, Rosa MariaDenaday, Lisandro RobertoBuldain, Graciela YolandaCampodallorto, VivianaCHLORINATED PHENOLSCOPPER COMPLEXHETEROGENEOUS CATALYSTPOLYAMPHOLYTEXPShttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1A complex between Cu(II) and a polyampholyte synthesized from methacrylic acid, imidazole and ethyleneglycol diglycidyl ether was used as a heterogeneous catalyst for hydrogen peroxide activation and degradation of chlorophenols. The material was characterized by XPS and by measurements of the zeta potential. The isoelectric point determined experimentally was 8.0, differing from that obtained by titration (6.4), which indicated the presence of fixed positive charges in disubstituted imidazole units. The XPS N 1s signal for pyridinic nitrogen in the imidazole units, and the O 1s signals from the carbonyl, hydroxyl and carboxylate groups shifted to higher binding energies after copper uptake, proving the chemical nature of Cu(II) adsorption on the polyampholyte. The XPS spectrum of the complex showed a Cu 2p3/2 peak at 934.7 eV and the characteristic shake-up satellite of Cu(II). When the complex was used as a heterogeneous catalyst for H2O2 activation, Cu(I) was proved to be a probable intermediate species and contributed to elucidate the mechanism. The Auger CuLMM spectrum supports the presence of Cu(I) with a kinetic energy value of 914.8 eV. The complex was applied in the oxidation of chlorinated phenols in aqueous solution at room temperature without any loss in efficiency. © 2011 Elsevier B.V. All rights reserved.Fil: Lazaro Martinez, Juan Manuel. Universidad de Buenos Aires. Facultad de Farmacia y Bioquímica. Departamento de Química Orgánica; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Rodríguez Castellón, Enrique. Universidad de Málaga; EspañaFil: Torres Sanchez, Rosa Maria. Provincia de Buenos Aires. Gobernación. Comisión de Investigaciones Científicas. Centro de Tecnología de Recursos Minerales y Cerámica. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Centro de Tecnología de Recursos Minerales y Cerámica; ArgentinaFil: Denaday, Lisandro Roberto. Universidad de Buenos Aires. Facultad de Farmacia y Bioquímica. Departamento de Química Analítica y Fisicoquímica; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Buldain, Graciela Yolanda. Universidad de Buenos Aires. Facultad de Farmacia y Bioquímica. Departamento de Química Orgánica; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Campodallorto, Viviana. Universidad de Buenos Aires. Facultad de Farmacia y Bioquímica. Departamento de Química Analítica y Fisicoquímica; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaElsevier Science2011-04-01info: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/11336/151987Lazaro Martinez, Juan Manuel; Rodríguez Castellón, Enrique; Torres Sanchez, Rosa Maria; Denaday, Lisandro Roberto; Buldain, Graciela Yolanda; et al.; XPS studies on the Cu(I,II)-polyampholyte heterogeneous catalyst: An insight into its structure and mechanism; Elsevier Science; Journal of Molecular Catalysis A: Chemical; 339; 1-2; 01-4-2011; 43-511381-1169CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1016/j.molcata.2011.02.010info:eu-repo/semantics/altIdentifier/url/https://linkinghub.elsevier.com/retrieve/pii/S1381116911000781info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T09:45:37Zoai:ri.conicet.gov.ar:11336/151987instacron: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 09:45:37.772CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv XPS studies on the Cu(I,II)-polyampholyte heterogeneous catalyst: An insight into its structure and mechanism
title XPS studies on the Cu(I,II)-polyampholyte heterogeneous catalyst: An insight into its structure and mechanism
spellingShingle XPS studies on the Cu(I,II)-polyampholyte heterogeneous catalyst: An insight into its structure and mechanism
Lazaro Martinez, Juan Manuel
CHLORINATED PHENOLS
COPPER COMPLEX
HETEROGENEOUS CATALYST
POLYAMPHOLYTE
XPS
title_short XPS studies on the Cu(I,II)-polyampholyte heterogeneous catalyst: An insight into its structure and mechanism
title_full XPS studies on the Cu(I,II)-polyampholyte heterogeneous catalyst: An insight into its structure and mechanism
title_fullStr XPS studies on the Cu(I,II)-polyampholyte heterogeneous catalyst: An insight into its structure and mechanism
title_full_unstemmed XPS studies on the Cu(I,II)-polyampholyte heterogeneous catalyst: An insight into its structure and mechanism
title_sort XPS studies on the Cu(I,II)-polyampholyte heterogeneous catalyst: An insight into its structure and mechanism
dc.creator.none.fl_str_mv Lazaro Martinez, Juan Manuel
Rodríguez Castellón, Enrique
Torres Sanchez, Rosa Maria
Denaday, Lisandro Roberto
Buldain, Graciela Yolanda
Campodallorto, Viviana
author Lazaro Martinez, Juan Manuel
author_facet Lazaro Martinez, Juan Manuel
Rodríguez Castellón, Enrique
Torres Sanchez, Rosa Maria
Denaday, Lisandro Roberto
Buldain, Graciela Yolanda
Campodallorto, Viviana
author_role author
author2 Rodríguez Castellón, Enrique
Torres Sanchez, Rosa Maria
Denaday, Lisandro Roberto
Buldain, Graciela Yolanda
Campodallorto, Viviana
author2_role author
author
author
author
author
dc.subject.none.fl_str_mv CHLORINATED PHENOLS
COPPER COMPLEX
HETEROGENEOUS CATALYST
POLYAMPHOLYTE
XPS
topic CHLORINATED PHENOLS
COPPER COMPLEX
HETEROGENEOUS CATALYST
POLYAMPHOLYTE
XPS
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv A complex between Cu(II) and a polyampholyte synthesized from methacrylic acid, imidazole and ethyleneglycol diglycidyl ether was used as a heterogeneous catalyst for hydrogen peroxide activation and degradation of chlorophenols. The material was characterized by XPS and by measurements of the zeta potential. The isoelectric point determined experimentally was 8.0, differing from that obtained by titration (6.4), which indicated the presence of fixed positive charges in disubstituted imidazole units. The XPS N 1s signal for pyridinic nitrogen in the imidazole units, and the O 1s signals from the carbonyl, hydroxyl and carboxylate groups shifted to higher binding energies after copper uptake, proving the chemical nature of Cu(II) adsorption on the polyampholyte. The XPS spectrum of the complex showed a Cu 2p3/2 peak at 934.7 eV and the characteristic shake-up satellite of Cu(II). When the complex was used as a heterogeneous catalyst for H2O2 activation, Cu(I) was proved to be a probable intermediate species and contributed to elucidate the mechanism. The Auger CuLMM spectrum supports the presence of Cu(I) with a kinetic energy value of 914.8 eV. The complex was applied in the oxidation of chlorinated phenols in aqueous solution at room temperature without any loss in efficiency. © 2011 Elsevier B.V. All rights reserved.
Fil: Lazaro Martinez, Juan Manuel. Universidad de Buenos Aires. Facultad de Farmacia y Bioquímica. Departamento de Química Orgánica; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Rodríguez Castellón, Enrique. Universidad de Málaga; España
Fil: Torres Sanchez, Rosa Maria. Provincia de Buenos Aires. Gobernación. Comisión de Investigaciones Científicas. Centro de Tecnología de Recursos Minerales y Cerámica. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Centro de Tecnología de Recursos Minerales y Cerámica; Argentina
Fil: Denaday, Lisandro Roberto. Universidad de Buenos Aires. Facultad de Farmacia y Bioquímica. Departamento de Química Analítica y Fisicoquímica; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Buldain, Graciela Yolanda. Universidad de Buenos Aires. Facultad de Farmacia y Bioquímica. Departamento de Química Orgánica; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Campodallorto, Viviana. Universidad de Buenos Aires. Facultad de Farmacia y Bioquímica. Departamento de Química Analítica y Fisicoquímica; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
description A complex between Cu(II) and a polyampholyte synthesized from methacrylic acid, imidazole and ethyleneglycol diglycidyl ether was used as a heterogeneous catalyst for hydrogen peroxide activation and degradation of chlorophenols. The material was characterized by XPS and by measurements of the zeta potential. The isoelectric point determined experimentally was 8.0, differing from that obtained by titration (6.4), which indicated the presence of fixed positive charges in disubstituted imidazole units. The XPS N 1s signal for pyridinic nitrogen in the imidazole units, and the O 1s signals from the carbonyl, hydroxyl and carboxylate groups shifted to higher binding energies after copper uptake, proving the chemical nature of Cu(II) adsorption on the polyampholyte. The XPS spectrum of the complex showed a Cu 2p3/2 peak at 934.7 eV and the characteristic shake-up satellite of Cu(II). When the complex was used as a heterogeneous catalyst for H2O2 activation, Cu(I) was proved to be a probable intermediate species and contributed to elucidate the mechanism. The Auger CuLMM spectrum supports the presence of Cu(I) with a kinetic energy value of 914.8 eV. The complex was applied in the oxidation of chlorinated phenols in aqueous solution at room temperature without any loss in efficiency. © 2011 Elsevier B.V. All rights reserved.
publishDate 2011
dc.date.none.fl_str_mv 2011-04-01
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/11336/151987
Lazaro Martinez, Juan Manuel; Rodríguez Castellón, Enrique; Torres Sanchez, Rosa Maria; Denaday, Lisandro Roberto; Buldain, Graciela Yolanda; et al.; XPS studies on the Cu(I,II)-polyampholyte heterogeneous catalyst: An insight into its structure and mechanism; Elsevier Science; Journal of Molecular Catalysis A: Chemical; 339; 1-2; 01-4-2011; 43-51
1381-1169
CONICET Digital
CONICET
url http://hdl.handle.net/11336/151987
identifier_str_mv Lazaro Martinez, Juan Manuel; Rodríguez Castellón, Enrique; Torres Sanchez, Rosa Maria; Denaday, Lisandro Roberto; Buldain, Graciela Yolanda; et al.; XPS studies on the Cu(I,II)-polyampholyte heterogeneous catalyst: An insight into its structure and mechanism; Elsevier Science; Journal of Molecular Catalysis A: Chemical; 339; 1-2; 01-4-2011; 43-51
1381-1169
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.molcata.2011.02.010
info:eu-repo/semantics/altIdentifier/url/https://linkinghub.elsevier.com/retrieve/pii/S1381116911000781
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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