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A Close Look at the Structure of the TiO2-APTES Interface in Hybrid Nanomaterials and Its Degradation Pathway: An Experimental and Theoretical Study.

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Title: A Close Look at the Structure of the TiO2-APTES Interface in Hybrid Nanomaterials and Its Degradation Pathway: An Experimental and Theoretical Study.
Authors: Meroni, Daniela1,2 daniela.meroni@unimi.it, Lo Presti, Leonardo1,3 leonardo.lopresti@unimi.it, Di Liberto, Giovanni1, Ceotto, Michele1,2 michele.ceotto@unimi.it, Acres, Robert G.4, Prince, Kevin C.5,6,7, Bellani, Roberto1, Soliveri, Guido8, Ardizzone, Silvia1,2
Source: Journal of Physical Chemistry B. Jan2017, Vol. 121 Issue 1, p430-440. 11p.
Subjects: Crystal structure, Titanium oxides, Nanostructured materials
Abstract: The surface functionalization of TiO2-based materials with alkylsilanes is attractive in several cutting-edge applications, such as photovoltaics, sensors, and nanocarriers for the controlled release of bioactive molecules. (3-Aminopropyl)triethoxysilane (APTES) is able to self-assemble to form monolayers on TiO2 surfaces, but its adsorption geometry and solar-induced photodegradation pathways are not well understood. We here employ advanced experimental (XPS, NEXAFS, AFM, HR-TEM, and FT-IR) and theoretical (plane-wave DFT) tools to investigate the preferential interaction mode of APTES on anatase TiO2. We demonstrate that monomeric APTES chemisorption should proceed through covalent Si-O-Ti bonds. Although dimerization of the silane through Si-O-Si bonds is possible, further polymerization on the surface is scarcely probable. Terminal amino groups are expected to be partially involved in strong charge-assisted hydrogen bonds with surface hydroxyl groups of TiO2, resulting in a reduced propensity to react with other species. Solar-induced mineralization proceeds through preferential cleavage of the alkyl groups, leading to the rapid loss of the terminal NH2 moieties, whereas the Si-bearing head of APTES undergoes slower oxidation and remains bound to the surface. The suitability of employing the silane as a linker with other chemical species is discussed in the context of controlled degradation of APTES monolayers for drug release and surface patterning. [ABSTRACT FROM AUTHOR]
Copyright of Journal of Physical Chemistry B is the property of American Chemical Society and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)
Database: Engineering Source
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Header DbId: egs
DbLabel: Engineering Source
An: 120741972
AccessLevel: 6
PubType: Academic Journal
PubTypeId: academicJournal
PreciseRelevancyScore: 0
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  Data: A Close Look at the Structure of the TiO<subscript>2</subscript>-APTES Interface in Hybrid Nanomaterials and Its Degradation Pathway: An Experimental and Theoretical Study.
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  Data: <searchLink fieldCode="AR" term="%22Meroni%2C+Daniela%22">Meroni, Daniela</searchLink><relatesTo>1,2</relatesTo><i> daniela.meroni@unimi.it</i><br /><searchLink fieldCode="AR" term="%22Lo+Presti%2C+Leonardo%22">Lo Presti, Leonardo</searchLink><relatesTo>1,3</relatesTo><i> leonardo.lopresti@unimi.it</i><br /><searchLink fieldCode="AR" term="%22Di+Liberto%2C+Giovanni%22">Di Liberto, Giovanni</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Ceotto%2C+Michele%22">Ceotto, Michele</searchLink><relatesTo>1,2</relatesTo><i> michele.ceotto@unimi.it</i><br /><searchLink fieldCode="AR" term="%22Acres%2C+Robert+G%2E%22">Acres, Robert G.</searchLink><relatesTo>4</relatesTo><br /><searchLink fieldCode="AR" term="%22Prince%2C+Kevin+C%2E%22">Prince, Kevin C.</searchLink><relatesTo>5,6,7</relatesTo><br /><searchLink fieldCode="AR" term="%22Bellani%2C+Roberto%22">Bellani, Roberto</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Soliveri%2C+Guido%22">Soliveri, Guido</searchLink><relatesTo>8</relatesTo><br /><searchLink fieldCode="AR" term="%22Ardizzone%2C+Silvia%22">Ardizzone, Silvia</searchLink><relatesTo>1,2</relatesTo>
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  Data: <searchLink fieldCode="JN" term="%22Journal+of+Physical+Chemistry+B%22">Journal of Physical Chemistry B</searchLink>. Jan2017, Vol. 121 Issue 1, p430-440. 11p.
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  Data: <searchLink fieldCode="DE" term="%22Crystal+structure%22">Crystal structure</searchLink><br /><searchLink fieldCode="DE" term="%22Titanium+oxides%22">Titanium oxides</searchLink><br /><searchLink fieldCode="DE" term="%22Nanostructured+materials%22">Nanostructured materials</searchLink>
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  Data: The surface functionalization of TiO2-based materials with alkylsilanes is attractive in several cutting-edge applications, such as photovoltaics, sensors, and nanocarriers for the controlled release of bioactive molecules. (3-Aminopropyl)triethoxysilane (APTES) is able to self-assemble to form monolayers on TiO2 surfaces, but its adsorption geometry and solar-induced photodegradation pathways are not well understood. We here employ advanced experimental (XPS, NEXAFS, AFM, HR-TEM, and FT-IR) and theoretical (plane-wave DFT) tools to investigate the preferential interaction mode of APTES on anatase TiO2. We demonstrate that monomeric APTES chemisorption should proceed through covalent Si-O-Ti bonds. Although dimerization of the silane through Si-O-Si bonds is possible, further polymerization on the surface is scarcely probable. Terminal amino groups are expected to be partially involved in strong charge-assisted hydrogen bonds with surface hydroxyl groups of TiO2, resulting in a reduced propensity to react with other species. Solar-induced mineralization proceeds through preferential cleavage of the alkyl groups, leading to the rapid loss of the terminal NH2 moieties, whereas the Si-bearing head of APTES undergoes slower oxidation and remains bound to the surface. The suitability of employing the silane as a linker with other chemical species is discussed in the context of controlled degradation of APTES monolayers for drug release and surface patterning. [ABSTRACT FROM AUTHOR]
– Name: AbstractSuppliedCopyright
  Label:
  Group: Ab
  Data: <i>Copyright of Journal of Physical Chemistry B is the property of American Chemical Society and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.)
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        Value: 10.1021/acs.jpcc.6b10720
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      – Code: eng
        Text: English
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        PageCount: 11
        StartPage: 430
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      – SubjectFull: Crystal structure
        Type: general
      – SubjectFull: Titanium oxides
        Type: general
      – SubjectFull: Nanostructured materials
        Type: general
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      – TitleFull: A Close Look at the Structure of the TiO2-APTES Interface in Hybrid Nanomaterials and Its Degradation Pathway: An Experimental and Theoretical Study.
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              M: 01
              Text: Jan2017
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              Y: 2017
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