Surface modification of TiO2 nanoparticles with AHAPS aminosilane: distinction between physisorption and chemisorption
Identifieur interne : 000491 ( Main/Exploration ); précédent : 000490; suivant : 000492Surface modification of TiO2 nanoparticles with AHAPS aminosilane: distinction between physisorption and chemisorption
Auteurs : Mounir Kassir [Liban] ; Thibault Roques-Carmes [France] ; Tayssir Hamieh [Liban] ; Angelina Razafitianamaharavo [France] ; Odile Barres [France] ; Joumana Toufaily [Liban] ; Frédéric Villiéras [France]Source :
- Adsorption - Journal of the International Adsorption Society [ 0929-5607 ] ; 2013-12.
English descriptors
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Abstract
This paper addresses the surface modification of TiO2 nanoparticles with n-(6-aminohexyl)aminopropyltrimethoxysilane (AHAPS) using various initial aminosilane concentrations. The main objective of this article is to show experimentally the importance of the physisorption during the grafting process. The distinction between chemisorbed and physisorbed aminosilane molecules on TiO2 is thoroughly analyzed. The surface of bare and modified TiO2 particles has been characterized by Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS) to gain a better understanding of the adsorption mechanism of AHAPS on TiO2. Quantitative information on surface energy of TiO2, in terms of adsorption energy sites and heterogeneity, has been investigated by quasi-equilibrium low-pressure adsorption technique using nitrogen and argon as probe molecules. The FTIR and XPS data are combined to estimate and discuss the chemisorbed and physisorbed contribution. The results demonstrate that both physisorption and chemisorption occurs but they display a different behavior. The physisorbed amounts are much higher than the chemisorbed amounts. This shows that the main part of the adsorbed layer is composed of physisorbed molecules. The physisorbed uptake depends highly on the AHAPS concentration while the chemisorbed amount remains constant. Quasi-equilibrium Ar derivative adsorption isotherms reveal that the AHAPS molecules are mostly located on the {101} and {001} faces of titania and that the two faces display the same reactivity toward AHAPS sorption. Nitrogen adsorption experiments show that the sorption takes place on the three polar surface sites of high energy. The molecules are chemisorbed onto the site displaying the highest energy while they are physisorbed on the two lower energy sites.
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DOI: 10.1007/s10450-013-9555-y
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CS 25233 - 54052 Nancy cedex</addrLine><country key="FR"></country></address><ref type="url">http://www.univ-lorraine.fr/</ref></desc></hal:affiliation><country>France</country></affiliation></author><author><name sortKey="Hamieh, Tayssir" sort="Hamieh, Tayssir" uniqKey="Hamieh T" first="Tayssir" last="Hamieh">Tayssir Hamieh</name><affiliation wicri:level="1"><hal:affiliation type="laboratory" xml:id="struct-407123" status="INCOMING"><orgName>Lab Mat Catalysis Environm & Analyt Methods, Beirut, Lebanon</orgName><desc><address><country key="LB"></country></address></desc><listRelation><relation active="#struct-249910" type="direct"></relation><relation active="#struct-359613" type="indirect"></relation></listRelation><tutelles><tutelle active="#struct-249910" type="direct"><org type="laboratory" xml:id="struct-249910" status="INCOMING"><orgName>Faculty of Science, Lebanese University</orgName><desc><address><addrLine>Beyrouth</addrLine><country key="LB"></country></address></desc><listRelation><relation active="#struct-359613" type="direct"></relation></listRelation></org></tutelle><tutelle active="#struct-359613" type="indirect"><org type="institution" xml:id="struct-359613" status="INCOMING"><orgName>Hadath Campus</orgName><desc><address><country key="FR"></country></address></desc></org></tutelle></tutelles></hal:affiliation><country>Liban</country></affiliation></author><author><name sortKey="Razafitianamaharavo, Angelina" sort="Razafitianamaharavo, Angelina" uniqKey="Razafitianamaharavo A" first="Angelina" last="Razafitianamaharavo">Angelina Razafitianamaharavo</name><affiliation wicri:level="1"><hal:affiliation type="laboratory" xml:id="struct-237201" status="VALID"><idno type="IdRef">174161565</idno><idno type="RNSR">201320576N</idno><idno type="IdUnivLorraine">[UL]RRI--</idno><orgName>Laboratoire Interdisciplinaire des Environnements Continentaux</orgName><orgName type="acronym">LIEC</orgName><date type="start">2013-01-01</date><desc><address><addrLine>Site Charmois : 15 Avenue du Charmois, F-54500 VANDOEUVRE-LES-NANCY ; Site Aiguillettes : Faculté des Sciences et Technologies, F-54506 VANDOEUVRE-LES-NANCY ; Site Bridoux : Campus Bridoux - Rue du Général Delestraint, F-57070 METZ ; Site Thionville : IUT de Thionville-Yutz - Espace Cormontaigne, F-57970 THIONVILLE-YUTZ</addrLine><country key="FR"></country></address><ref type="url">http://liec.univ-lorraine.fr/</ref></desc><listRelation><relation active="#struct-413289" type="direct"></relation><relation name="UMR7360" active="#struct-441569" type="direct"></relation></listRelation><tutelles><tutelle active="#struct-413289" type="direct"><org type="institution" xml:id="struct-413289" status="VALID"><idno type="IdRef">157040569</idno><idno type="IdUnivLorraine">[UL]100--</idno><orgName>Université de Lorraine</orgName><orgName type="acronym">UL</orgName><date type="start">2012-01-01</date><desc><address><addrLine>34 cours Léopold - CS 25233 - 54052 Nancy cedex</addrLine><country key="FR"></country></address><ref type="url">http://www.univ-lorraine.fr/</ref></desc></org></tutelle><tutelle name="UMR7360" active="#struct-441569" type="direct"><org type="institution" xml:id="struct-441569" status="VALID"><idno type="ISNI">0000000122597504</idno><idno type="IdRef">02636817X</idno><orgName>Centre National de la Recherche Scientifique</orgName><orgName type="acronym">CNRS</orgName><date type="start">1939-10-19</date><desc><address><country key="FR"></country></address><ref type="url">http://www.cnrs.fr/</ref></desc></org></tutelle></tutelles></hal:affiliation><country>France</country><placeName><settlement type="city">Nancy</settlement><settlement type="city">Metz</settlement><region type="region" nuts="2">Grand Est</region><region type="old region" nuts="2">Lorraine (région)</region></placeName><orgName type="university">Université de Lorraine</orgName></affiliation></author><author><name sortKey="Barres, Odile" sort="Barres, Odile" uniqKey="Barres O" first="Odile" last="Barres">Odile Barres</name><affiliation wicri:level="1"><hal:affiliation type="institution" xml:id="struct-320707" status="VALID"><orgName>Centre de recherches sur la géologie des matières premières minérales et énergétiques</orgName><orgName type="acronym">CREGU</orgName><desc><address><addrLine>BP 20023, 54501 Vandoeuvre-lès-Nancy cedex, France</addrLine><country key="FR"></country></address></desc></hal:affiliation><country>France</country></affiliation></author><author><name sortKey="Toufaily, Joumana" sort="Toufaily, Joumana" uniqKey="Toufaily J" first="Joumana" last="Toufaily">Joumana Toufaily</name><affiliation wicri:level="1"><hal:affiliation type="laboratory" xml:id="struct-407123" status="INCOMING"><orgName>Lab Mat Catalysis Environm & Analyt Methods, Beirut, Lebanon</orgName><desc><address><country key="LB"></country></address></desc><listRelation><relation active="#struct-249910" type="direct"></relation><relation active="#struct-359613" type="indirect"></relation></listRelation><tutelles><tutelle active="#struct-249910" type="direct"><org type="laboratory" xml:id="struct-249910" status="INCOMING"><orgName>Faculty of Science, Lebanese University</orgName><desc><address><addrLine>Beyrouth</addrLine><country key="LB"></country></address></desc><listRelation><relation active="#struct-359613" type="direct"></relation></listRelation></org></tutelle><tutelle active="#struct-359613" type="indirect"><org type="institution" xml:id="struct-359613" status="INCOMING"><orgName>Hadath Campus</orgName><desc><address><country key="FR"></country></address></desc></org></tutelle></tutelles></hal:affiliation><country>Liban</country></affiliation></author><author><name sortKey="Villieras, Frederic" sort="Villieras, Frederic" uniqKey="Villieras F" first="Frédéric" last="Villiéras">Frédéric Villiéras</name><affiliation wicri:level="1"><hal:affiliation type="laboratory" xml:id="struct-237201" status="VALID"><idno type="IdRef">174161565</idno><idno type="RNSR">201320576N</idno><idno type="IdUnivLorraine">[UL]RRI--</idno><orgName>Laboratoire Interdisciplinaire des Environnements Continentaux</orgName><orgName type="acronym">LIEC</orgName><date type="start">2013-01-01</date><desc><address><addrLine>Site Charmois : 15 Avenue du Charmois, F-54500 VANDOEUVRE-LES-NANCY ; Site Aiguillettes : Faculté des Sciences et Technologies, F-54506 VANDOEUVRE-LES-NANCY ; Site Bridoux : Campus Bridoux - Rue du Général Delestraint, F-57070 METZ ; Site Thionville : IUT de Thionville-Yutz - Espace Cormontaigne, F-57970 THIONVILLE-YUTZ</addrLine><country key="FR"></country></address><ref type="url">http://liec.univ-lorraine.fr/</ref></desc><listRelation><relation active="#struct-413289" type="direct"></relation><relation name="UMR7360" active="#struct-441569" type="direct"></relation></listRelation><tutelles><tutelle active="#struct-413289" type="direct"><org type="institution" xml:id="struct-413289" status="VALID"><idno type="IdRef">157040569</idno><idno type="IdUnivLorraine">[UL]100--</idno><orgName>Université de Lorraine</orgName><orgName type="acronym">UL</orgName><date type="start">2012-01-01</date><desc><address><addrLine>34 cours Léopold - CS 25233 - 54052 Nancy cedex</addrLine><country key="FR"></country></address><ref type="url">http://www.univ-lorraine.fr/</ref></desc></org></tutelle><tutelle name="UMR7360" active="#struct-441569" type="direct"><org type="institution" xml:id="struct-441569" status="VALID"><idno type="ISNI">0000000122597504</idno><idno type="IdRef">02636817X</idno><orgName>Centre National de la Recherche Scientifique</orgName><orgName type="acronym">CNRS</orgName><date type="start">1939-10-19</date><desc><address><country key="FR"></country></address><ref type="url">http://www.cnrs.fr/</ref></desc></org></tutelle></tutelles></hal:affiliation><country>France</country><placeName><settlement type="city">Nancy</settlement><settlement type="city">Metz</settlement><region type="region" nuts="2">Grand Est</region><region type="old region" nuts="2">Lorraine (région)</region></placeName><orgName type="university">Université de Lorraine</orgName></affiliation></author></analytic><idno type="DOI">10.1007/s10450-013-9555-y</idno><series><title level="j">Adsorption - Journal of the International Adsorption Society</title><idno type="ISSN">0929-5607</idno><imprint><date type="datePub">2013-12</date></imprint></series></biblStruct></sourceDesc></fileDesc><profileDesc><textClass><keywords scheme="mix" xml:lang="en"><term>Aminosilane coupling agent</term><term>Chemisorption</term><term>Low-pressure argon and nitrogen adsorption</term><term>Physisorption</term><term>Surface modification</term><term>TiO2 nanoparticles</term></keywords></textClass></profileDesc></teiHeader><front><div type="abstract" xml:lang="en">This paper addresses the surface modification of TiO2 nanoparticles with n-(6-aminohexyl)aminopropyltrimethoxysilane (AHAPS) using various initial aminosilane concentrations. The main objective of this article is to show experimentally the importance of the physisorption during the grafting process. The distinction between chemisorbed and physisorbed aminosilane molecules on TiO2 is thoroughly analyzed. The surface of bare and modified TiO2 particles has been characterized by Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS) to gain a better understanding of the adsorption mechanism of AHAPS on TiO2. Quantitative information on surface energy of TiO2, in terms of adsorption energy sites and heterogeneity, has been investigated by quasi-equilibrium low-pressure adsorption technique using nitrogen and argon as probe molecules. The FTIR and XPS data are combined to estimate and discuss the chemisorbed and physisorbed contribution. The results demonstrate that both physisorption and chemisorption occurs but they display a different behavior. The physisorbed amounts are much higher than the chemisorbed amounts. This shows that the main part of the adsorbed layer is composed of physisorbed molecules. The physisorbed uptake depends highly on the AHAPS concentration while the chemisorbed amount remains constant. Quasi-equilibrium Ar derivative adsorption isotherms reveal that the AHAPS molecules are mostly located on the {101} and {001} faces of titania and that the two faces display the same reactivity toward AHAPS sorption. Nitrogen adsorption experiments show that the sorption takes place on the three polar surface sites of high energy. The molecules are chemisorbed onto the site displaying the highest energy while they are physisorbed on the two lower energy sites.</div></front></TEI><affiliations><list><country><li>France</li><li>Liban</li></country><region><li>Grand Est</li><li>Lorraine (région)</li></region><settlement><li>Metz</li><li>Nancy</li></settlement><orgName><li>Université de Lorraine</li></orgName></list><tree><country name="Liban"><noRegion><name sortKey="Kassir, Mounir" sort="Kassir, Mounir" uniqKey="Kassir M" first="Mounir" last="Kassir">Mounir Kassir</name></noRegion><name sortKey="Hamieh, Tayssir" sort="Hamieh, Tayssir" uniqKey="Hamieh T" first="Tayssir" last="Hamieh">Tayssir Hamieh</name><name sortKey="Toufaily, Joumana" sort="Toufaily, Joumana" uniqKey="Toufaily J" first="Joumana" last="Toufaily">Joumana Toufaily</name></country><country name="France"><noRegion><name sortKey="Roques Carmes, Thibault" sort="Roques Carmes, Thibault" uniqKey="Roques Carmes T" first="Thibault" last="Roques-Carmes">Thibault Roques-Carmes</name></noRegion><name sortKey="Barres, Odile" sort="Barres, Odile" uniqKey="Barres O" first="Odile" last="Barres">Odile Barres</name><name sortKey="Razafitianamaharavo, Angelina" sort="Razafitianamaharavo, Angelina" uniqKey="Razafitianamaharavo A" first="Angelina" last="Razafitianamaharavo">Angelina Razafitianamaharavo</name><name sortKey="Villieras, Frederic" sort="Villieras, Frederic" uniqKey="Villieras F" first="Frédéric" last="Villiéras">Frédéric Villiéras</name></country></tree></affiliations></record>Pour manipuler ce document sous Unix (Dilib)
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