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

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 a...

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Autores principales: Calvo, A., Angelomé, P.C., Sánchez, V.M., Scherlis, D.A., Williams, F.J., Soler-Illia, G.J.A.A.
Formato: JOUR
Materias:
Amines
Thin films
Aminopropyl
Functionalized
Hybrid thin films
Mesoporous
Thick films
Acceso en línea:http://hdl.handle.net/20.500.12110/paper_08974756_v20_n14_p4661_Calvo
Aporte de:
Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA) de Universidad de Buenos Aires
id todo:paper_08974756_v20_n14_p4661_Calvo
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spelling todo:paper_08974756_v20_n14_p4661_Calvo2023-10-03T15:43:51Z Mesoporous aminopropyl-functionalized hybrid thin films with modulable surface and environment-responsive behavior Calvo, A. Angelomé, P.C. Sánchez, V.M. Scherlis, D.A. Williams, F.J. Soler-Illia, G.J.A.A. Amines Thin films Aminopropyl Functionalized Hybrid thin films Mesoporous Thick films 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. © 2008 American Chemical Society. Fil:Angelomé, P.C. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. Fil:Sánchez, V.M. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. Fil:Williams, F.J. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. Fil:Soler-Illia, G.J.A.A. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. JOUR info:eu-repo/semantics/openAccess http://creativecommons.org/licenses/by/2.5/ar http://hdl.handle.net/20.500.12110/paper_08974756_v20_n14_p4661_Calvo
institution Universidad de Buenos Aires
institution_str I-28
repository_str R-134
collection Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA)
topic Amines
Thin films
Aminopropyl
Functionalized
Hybrid thin films
Mesoporous
Thick films
spellingShingle Amines
Thin films
Aminopropyl
Functionalized
Hybrid thin films
Mesoporous
Thick films
Calvo, A.
Angelomé, P.C.
Sánchez, V.M.
Scherlis, D.A.
Williams, F.J.
Soler-Illia, G.J.A.A.
Mesoporous aminopropyl-functionalized hybrid thin films with modulable surface and environment-responsive behavior
topic_facet Amines
Thin films
Aminopropyl
Functionalized
Hybrid thin films
Mesoporous
Thick films
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. © 2008 American Chemical Society.
format JOUR
author Calvo, A.
Angelomé, P.C.
Sánchez, V.M.
Scherlis, D.A.
Williams, F.J.
Soler-Illia, G.J.A.A.
author_facet Calvo, A.
Angelomé, P.C.
Sánchez, V.M.
Scherlis, D.A.
Williams, F.J.
Soler-Illia, G.J.A.A.
author_sort Calvo, A.
title Mesoporous aminopropyl-functionalized hybrid thin films with modulable surface and environment-responsive behavior
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
url http://hdl.handle.net/20.500.12110/paper_08974756_v20_n14_p4661_Calvo
work_keys_str_mv AT calvoa mesoporousaminopropylfunctionalizedhybridthinfilmswithmodulablesurfaceandenvironmentresponsivebehavior
AT angelomepc mesoporousaminopropylfunctionalizedhybridthinfilmswithmodulablesurfaceandenvironmentresponsivebehavior
AT sanchezvm mesoporousaminopropylfunctionalizedhybridthinfilmswithmodulablesurfaceandenvironmentresponsivebehavior
AT scherlisda mesoporousaminopropylfunctionalizedhybridthinfilmswithmodulablesurfaceandenvironmentresponsivebehavior
AT williamsfj mesoporousaminopropylfunctionalizedhybridthinfilmswithmodulablesurfaceandenvironmentresponsivebehavior
AT solerilliagjaa mesoporousaminopropylfunctionalizedhybridthinfilmswithmodulablesurfaceandenvironmentresponsivebehavior
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