Mesoporous aminopropyl-functionalized hybrid thin films with modulable surface and environment-responsive behavior

Autores
Calvo, Alejandra; Angelome, Paula Cecilia; Sanchez, Veronica Muriel; Scherlis Perel, Damian Ariel; Williams, Federico José; Soler Illia, Galo Juan de Avila Arturo
Año de publicación
2008
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
A first study of the behavior of amino functions in mesoporous hybrid thin films M1-x(Si-(CH2)3NH2) xO2-x/2 (M = Si, Ti, Zr; 0.05 ≤ x ≤ 0.2) with accessible Im3̄m- or Fm3̄m-derived pore mesostructures is presented. An XPS study of surface nitrogen species shows two different sites corresponding to amino and ammonium groups. The ratio of these species changes with pH and is related to the nature of M, suggesting that the interaction between the organic functions and the surface M-OH groups can be tailored to tune the surface acid-base behavior. Density functional theory (DFT) calculations were used to rationalize the XPS observations showing that -NH3 + functions irreversibly transfer a proton to neighboring M-O- surface groups. The acid-base surface properties can be further modified by adding a phosphonate "capping" on the M surface sites. Our findings have a series of interesting implications in surface functionalization: attachment of biomolecules to surfaces, design of perm-selective or philicity-selective membranes, or design of catalysts that show a well-defined organic reactive function near surface hydroxyl groups.
Fil: Calvo, Alejandra. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina
Fil: Angelome, Paula Cecilia. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina
Fil: Sanchez, Veronica Muriel. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Departamento de Química Inorgánica, Analítica y Química Física; Argentina
Fil: Scherlis Perel, Damian Ariel. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Departamento de Química Inorgánica, Analítica y Química Física; Argentina
Fil: Williams, Federico José. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación en Nanociencia y Nanotecnología; Argentina
Fil: Soler Illia, Galo Juan de Avila Arturo. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación en Nanociencia y Nanotecnología; Argentina
Materia
Porous Materials
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:11336/74531
Acceder
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oai_identifier_str oai:ri.conicet.gov.ar:11336/74531
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Mesoporous aminopropyl-functionalized hybrid thin films with modulable surface and environment-responsive behaviorCalvo, AlejandraAngelome, Paula CeciliaSanchez, Veronica MurielScherlis Perel, Damian ArielWilliams, Federico JoséSoler Illia, Galo Juan de Avila ArturoPorous Materialshttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1A first study of the behavior of amino functions in mesoporous hybrid thin films M1-x(Si-(CH2)3NH2) xO2-x/2 (M = Si, Ti, Zr; 0.05 ≤ x ≤ 0.2) with accessible Im3̄m- or Fm3̄m-derived pore mesostructures is presented. An XPS study of surface nitrogen species shows two different sites corresponding to amino and ammonium groups. The ratio of these species changes with pH and is related to the nature of M, suggesting that the interaction between the organic functions and the surface M-OH groups can be tailored to tune the surface acid-base behavior. Density functional theory (DFT) calculations were used to rationalize the XPS observations showing that -NH3 + functions irreversibly transfer a proton to neighboring M-O- surface groups. The acid-base surface properties can be further modified by adding a phosphonate "capping" on the M surface sites. Our findings have a series of interesting implications in surface functionalization: attachment of biomolecules to surfaces, design of perm-selective or philicity-selective membranes, or design of catalysts that show a well-defined organic reactive function near surface hydroxyl groups.Fil: Calvo, Alejandra. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; ArgentinaFil: Angelome, Paula Cecilia. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; ArgentinaFil: Sanchez, Veronica Muriel. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Departamento de Química Inorgánica, Analítica y Química Física; ArgentinaFil: Scherlis Perel, Damian Ariel. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Departamento de Química Inorgánica, Analítica y Química Física; ArgentinaFil: Williams, Federico José. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación en Nanociencia y Nanotecnología; ArgentinaFil: Soler Illia, Galo Juan de Avila Arturo. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación en Nanociencia y Nanotecnología; ArgentinaAmerican Chemical Society2008-07info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/74531Calvo, Alejandra; Angelome, Paula Cecilia; Sanchez, Veronica Muriel; Scherlis Perel, Damian Ariel; Williams, Federico José; et al.; Mesoporous aminopropyl-functionalized hybrid thin films with modulable surface and environment-responsive behavior; American Chemical Society; Chemistry Of Materials; 20; 14; 7-2008; 4661-46680897-4756CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1021/cm800597kinfo:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/cm800597kinfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-22T11:42:38Zoai:ri.conicet.gov.ar:11336/74531instacron: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:34982025-10-22 11:42:38.413CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Mesoporous aminopropyl-functionalized hybrid thin films with modulable surface and environment-responsive behavior
title Mesoporous aminopropyl-functionalized hybrid thin films with modulable surface and environment-responsive behavior
spellingShingle Mesoporous aminopropyl-functionalized hybrid thin films with modulable surface and environment-responsive behavior
Calvo, Alejandra
Porous Materials
title_short Mesoporous aminopropyl-functionalized hybrid thin films with modulable surface and environment-responsive behavior
title_full Mesoporous aminopropyl-functionalized hybrid thin films with modulable surface and environment-responsive behavior
title_fullStr Mesoporous aminopropyl-functionalized hybrid thin films with modulable surface and environment-responsive behavior
title_full_unstemmed Mesoporous aminopropyl-functionalized hybrid thin films with modulable surface and environment-responsive behavior
title_sort Mesoporous aminopropyl-functionalized hybrid thin films with modulable surface and environment-responsive behavior
dc.creator.none.fl_str_mv Calvo, Alejandra
Angelome, Paula Cecilia
Sanchez, Veronica Muriel
Scherlis Perel, Damian Ariel
Williams, Federico José
Soler Illia, Galo Juan de Avila Arturo
author Calvo, Alejandra
author_facet Calvo, Alejandra
Angelome, Paula Cecilia
Sanchez, Veronica Muriel
Scherlis Perel, Damian Ariel
Williams, Federico José
Soler Illia, Galo Juan de Avila Arturo
author_role author
author2 Angelome, Paula Cecilia
Sanchez, Veronica Muriel
Scherlis Perel, Damian Ariel
Williams, Federico José
Soler Illia, Galo Juan de Avila Arturo
author2_role author
author
author
author
author
dc.subject.none.fl_str_mv Porous Materials
topic Porous Materials
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 first study of the behavior of amino functions in mesoporous hybrid thin films M1-x(Si-(CH2)3NH2) xO2-x/2 (M = Si, Ti, Zr; 0.05 ≤ x ≤ 0.2) with accessible Im3̄m- or Fm3̄m-derived pore mesostructures is presented. An XPS study of surface nitrogen species shows two different sites corresponding to amino and ammonium groups. The ratio of these species changes with pH and is related to the nature of M, suggesting that the interaction between the organic functions and the surface M-OH groups can be tailored to tune the surface acid-base behavior. Density functional theory (DFT) calculations were used to rationalize the XPS observations showing that -NH3 + functions irreversibly transfer a proton to neighboring M-O- surface groups. The acid-base surface properties can be further modified by adding a phosphonate "capping" on the M surface sites. Our findings have a series of interesting implications in surface functionalization: attachment of biomolecules to surfaces, design of perm-selective or philicity-selective membranes, or design of catalysts that show a well-defined organic reactive function near surface hydroxyl groups.
Fil: Calvo, Alejandra. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina
Fil: Angelome, Paula Cecilia. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina
Fil: Sanchez, Veronica Muriel. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Departamento de Química Inorgánica, Analítica y Química Física; Argentina
Fil: Scherlis Perel, Damian Ariel. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Departamento de Química Inorgánica, Analítica y Química Física; Argentina
Fil: Williams, Federico José. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación en Nanociencia y Nanotecnología; Argentina
Fil: Soler Illia, Galo Juan de Avila Arturo. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina. Comisión Nacional de Energía Atómica. Centro Atómico Constituyentes; Argentina. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación en Nanociencia y Nanotecnología; Argentina
description A first study of the behavior of amino functions in mesoporous hybrid thin films M1-x(Si-(CH2)3NH2) xO2-x/2 (M = Si, Ti, Zr; 0.05 ≤ x ≤ 0.2) with accessible Im3̄m- or Fm3̄m-derived pore mesostructures is presented. An XPS study of surface nitrogen species shows two different sites corresponding to amino and ammonium groups. The ratio of these species changes with pH and is related to the nature of M, suggesting that the interaction between the organic functions and the surface M-OH groups can be tailored to tune the surface acid-base behavior. Density functional theory (DFT) calculations were used to rationalize the XPS observations showing that -NH3 + functions irreversibly transfer a proton to neighboring M-O- surface groups. The acid-base surface properties can be further modified by adding a phosphonate "capping" on the M surface sites. Our findings have a series of interesting implications in surface functionalization: attachment of biomolecules to surfaces, design of perm-selective or philicity-selective membranes, or design of catalysts that show a well-defined organic reactive function near surface hydroxyl groups.
publishDate 2008
dc.date.none.fl_str_mv 2008-07
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/11336/74531
Calvo, Alejandra; Angelome, Paula Cecilia; Sanchez, Veronica Muriel; Scherlis Perel, Damian Ariel; Williams, Federico José; et al.; Mesoporous aminopropyl-functionalized hybrid thin films with modulable surface and environment-responsive behavior; American Chemical Society; Chemistry Of Materials; 20; 14; 7-2008; 4661-4668
0897-4756
CONICET Digital
CONICET
url http://hdl.handle.net/11336/74531
identifier_str_mv Calvo, Alejandra; Angelome, Paula Cecilia; Sanchez, Veronica Muriel; Scherlis Perel, Damian Ariel; Williams, Federico José; et al.; Mesoporous aminopropyl-functionalized hybrid thin films with modulable surface and environment-responsive behavior; American Chemical Society; Chemistry Of Materials; 20; 14; 7-2008; 4661-4668
0897-4756
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1021/cm800597k
info:eu-repo/semantics/altIdentifier/url/https://pubs.acs.org/doi/10.1021/cm800597k
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
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
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score 12.982451

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