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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2008
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Acceso en línea: | https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_08974756_v20_n14_p4661_Calvo http://hdl.handle.net/20.500.12110/paper_08974756_v20_n14_p4661_Calvo |
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paper:paper_08974756_v20_n14_p4661_Calvo2023-06-08T15:49:17Z Mesoporous aminopropyl-functionalized hybrid thin films with modulable surface and environment-responsive behavior Angelomé, Paula C. Sánchez, Verónica Muriel Williams, Federico Jose Soler Illia, Galo Juan de Avila Arturo 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. 2008 https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_08974756_v20_n14_p4661_Calvo 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 Angelomé, Paula C. Sánchez, Verónica Muriel Williams, Federico Jose Soler Illia, Galo Juan de Avila Arturo 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. |
author |
Angelomé, Paula C. Sánchez, Verónica Muriel Williams, Federico Jose Soler Illia, Galo Juan de Avila Arturo |
author_facet |
Angelomé, Paula C. Sánchez, Verónica Muriel Williams, Federico Jose Soler Illia, Galo Juan de Avila Arturo |
author_sort |
Angelomé, Paula C. |
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 |
publishDate |
2008 |
url |
https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_08974756_v20_n14_p4661_Calvo http://hdl.handle.net/20.500.12110/paper_08974756_v20_n14_p4661_Calvo |
work_keys_str_mv |
AT angelomepaulac mesoporousaminopropylfunctionalizedhybridthinfilmswithmodulablesurfaceandenvironmentresponsivebehavior AT sanchezveronicamuriel mesoporousaminopropylfunctionalizedhybridthinfilmswithmodulablesurfaceandenvironmentresponsivebehavior AT williamsfedericojose mesoporousaminopropylfunctionalizedhybridthinfilmswithmodulablesurfaceandenvironmentresponsivebehavior AT solerilliagalojuandeavilaarturo mesoporousaminopropylfunctionalizedhybridthinfilmswithmodulablesurfaceandenvironmentresponsivebehavior |
_version_ |
1768546634120036352 |