Abstract:
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.
Registro:
Documento: |
Artículo
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Título: | Mesoporous aminopropyl-functionalized hybrid thin films with modulable surface and environment-responsive behavior |
Autor: | Calvo, A.; Angelomé, P.C.; Sánchez, V.M.; Scherlis, D.A.; Williams, F.J.; Soler-Illia, G.J.A.A. |
Filiación: | Gerencia de Química, CNEA, Centro Atómico Constituyentes, Av. Gral Paz 1499, San Martín B1650KNA, Buenos Aires, Argentina DQIAyQF, FCEN, Pabellón II, C1428EHA Buenos Aires, Argentina CONICET, Av. Rivadavia 1917, C1033AAJ Buenos Aires, Argentina Departamento de Química de Superficies y Recubrimientos, TENARIS, Simini 250, B2804MHA Campana, Buenos Aires, Argentina Centro Interdisciplinario de Nanociencia y Nanotecnología, Av. Rivadavia 1917, C1033AAJ Buenos Aires, Argentina
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Palabras clave: | Amines; Thin films; Aminopropyl; Functionalized; Hybrid thin films; Mesoporous; Thick films |
Año: | 2008
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Volumen: | 20
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Número: | 14
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Página de inicio: | 4661
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Página de fin: | 4668
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DOI: |
http://dx.doi.org/10.1021/cm800597k |
Título revista: | Chemistry of Materials
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Título revista abreviado: | Chem. Mater.
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ISSN: | 08974756
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CODEN: | CMATE
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Registro: | https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_08974756_v20_n14_p4661_Calvo |
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Citas:
---------- APA ----------
Calvo, A., Angelomé, P.C., Sánchez, V.M., Scherlis, D.A., Williams, F.J. & Soler-Illia, G.J.A.A.
(2008)
. Mesoporous aminopropyl-functionalized hybrid thin films with modulable surface and environment-responsive behavior. Chemistry of Materials, 20(14), 4661-4668.
http://dx.doi.org/10.1021/cm800597k---------- CHICAGO ----------
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"
. Chemistry of Materials 20, no. 14
(2008) : 4661-4668.
http://dx.doi.org/10.1021/cm800597k---------- MLA ----------
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"
. Chemistry of Materials, vol. 20, no. 14, 2008, pp. 4661-4668.
http://dx.doi.org/10.1021/cm800597k---------- VANCOUVER ----------
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. Chem. Mater. 2008;20(14):4661-4668.
http://dx.doi.org/10.1021/cm800597k