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
- Institución
- Consejo Nacional de Investigaciones Científicas y Técnicas
- OAI Identificador
- oai:ri.conicet.gov.ar:11336/74531
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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 Técnicas2025-09-29T10:12:46Zoai: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:34982025-09-29 10:12:47.277CONICET 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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1844614037467299840 |
score |
13.070432 |