Characterization and comparison of the activity of boron-modified Co/TiO2 catalysts in butan-2-ol conversion and oxidative dehydrogenation of ethane
Identifieur interne : 000259 ( France/Analysis ); précédent : 000258; suivant : 000260Characterization and comparison of the activity of boron-modified Co/TiO2 catalysts in butan-2-ol conversion and oxidative dehydrogenation of ethane
Auteurs : Younes Brik [Maroc, France] ; Mohamed Kacimi [Maroc] ; Francois Bozon-Verduraz [France] ; Mahfoud Ziyad [Maroc]Source :
- Journal of catalysis : (Print) [ 0021-9517 ] ; 2002.
Descripteurs français
- Pascal (Inist)
- Wicri :
- topic : Cobalt, Hydrocarbure.
English descriptors
- KwdEn :
Abstract
Cobalt- and cobalt-boron-loaded TiO2 (anatase) catalysts were prepared and characterized before and after catalytic tests by XRD, HRTEM, IR, UV-visible, and laser Raman spectroscopy. Their activity was investigated in oxidative dehydrogenation (ODH) of ethane. In the absence of boron, the best performances were exhibited by the sample containing 7.6 wt% Co, which was selected for further investigations. At 550 °C, it displayed a stationary state with a conversion of 22.2% and an ethylene selectivity around 60%. This catalyst also showed in the first 3 h on stream a 30% decay in activity that was attributed to a concomitant loss of specific surface area and the formation of CoTiO3 and Co2TiO4 phases. The addition of 0.25 wt% boron to this Co(7.6)/TiO2 sample improved the ethane conversion and the ethylene selectivity, which attained 28.4 and 67%, respectively. Boron concentrations superior to 0.25 wt% negatively affected the catalysts performances, probably because at high loadings it profoundly modified the acid-base properties of the surface. XRD and HRTEM analyses showed that at the same time the size of Co3O4 crystallites decreased. IR investigations confirmed the increase in acidity upon boron addition and the decrease in strength of the basic sites which were involved in the dehydrogenation processes. The catalytic behavior and the acid-base properties of Co(7.6)/TiO2 loaded with different amounts of boron were also studied using butan-2-ol conversion. Boron addition enhanced the dehydration and the dehydrogenation reactions. However, above 0.25 wt% it decreased the dehydrogenation activity, confirming the modifications of the properties of the acid-base centers revealed by the IR studies. For this optimal concentration of boron, the activity and the selectivity in butan-2-ol dehydrogenation exhibited a maximum that coincided with the one observed in the ethane ODH, which suggests that both reactions possibly involved the same type of active centers.
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P. 1014</s1><s2>Rabat</s2><s3>MAR</s3><sZ>1 aut.</sZ><sZ>2 aut.</sZ><sZ>4 aut.</sZ></inist:fA14><country>Maroc</country><placeName><settlement type="city">Rabat</settlement><region nuts="2">Rabat-Salé-Kénitra</region></placeName></affiliation><affiliation wicri:level="3"><inist:fA14 i1="02"><s1>Laboratoire de Chimie des Matériaux Divisés et Catalyse, Université Paris 7, 2 place Jussieu</s1><s2>75251 Paris</s2><s3>FRA</s3><sZ>1 aut.</sZ><sZ>3 aut.</sZ></inist:fA14><country>France</country><placeName><region type="region" nuts="2">Île-de-France</region><settlement type="city">Paris</settlement></placeName></affiliation></author><author><name sortKey="Kacimi, Mohamed" sort="Kacimi, Mohamed" uniqKey="Kacimi M" first="Mohamed" last="Kacimi">Mohamed Kacimi</name><affiliation wicri:level="3"><inist:fA14 i1="01"><s1>Faculté des Sciences, Département de Chimie, Laboratoire de Physico-chimie des Matériaux et Catalyse, Avenue Ibn Battouta, B. P. 1014</s1><s2>Rabat</s2><s3>MAR</s3><sZ>1 aut.</sZ><sZ>2 aut.</sZ><sZ>4 aut.</sZ></inist:fA14><country>Maroc</country><placeName><settlement type="city">Rabat</settlement><region nuts="2">Rabat-Salé-Kénitra</region></placeName></affiliation></author><author><name sortKey="Bozon Verduraz, Francois" sort="Bozon Verduraz, Francois" uniqKey="Bozon Verduraz F" first="Francois" last="Bozon-Verduraz">Francois Bozon-Verduraz</name><affiliation wicri:level="3"><inist:fA14 i1="02"><s1>Laboratoire de Chimie des Matériaux Divisés et Catalyse, Université Paris 7, 2 place Jussieu</s1><s2>75251 Paris</s2><s3>FRA</s3><sZ>1 aut.</sZ><sZ>3 aut.</sZ></inist:fA14><country>France</country><placeName><region type="region" nuts="2">Île-de-France</region><settlement type="city">Paris</settlement></placeName></affiliation></author><author><name sortKey="Ziyad, Mahfoud" sort="Ziyad, Mahfoud" uniqKey="Ziyad M" first="Mahfoud" last="Ziyad">Mahfoud Ziyad</name><affiliation wicri:level="3"><inist:fA14 i1="01"><s1>Faculté des Sciences, Département de Chimie, Laboratoire de Physico-chimie des Matériaux et Catalyse, Avenue Ibn Battouta, B. P. 1014</s1><s2>Rabat</s2><s3>MAR</s3><sZ>1 aut.</sZ><sZ>2 aut.</sZ><sZ>4 aut.</sZ></inist:fA14><country>Maroc</country><placeName><settlement type="city">Rabat</settlement><region nuts="2">Rabat-Salé-Kénitra</region></placeName></affiliation></author></analytic><series><title level="j" type="main">Journal of catalysis : (Print)</title><title level="j" type="abbreviated">J. catal. : (Print)</title><idno type="ISSN">0021-9517</idno><imprint><date when="2002">2002</date></imprint></series></biblStruct></sourceDesc><seriesStmt><title level="j" type="main">Journal of catalysis : (Print)</title><title level="j" type="abbreviated">J. catal. : (Print)</title><idno type="ISSN">0021-9517</idno></seriesStmt></fileDesc><profileDesc><textClass><keywords scheme="KwdEn" xml:lang="en"><term>Alkane</term><term>Boron</term><term>Butanol</term><term>Catalytic reaction</term><term>Cobalt</term><term>Dehydrogenation</term><term>Ethane</term><term>Experimental study</term><term>Heterogeneous catalysis</term><term>Hydrocarbon</term><term>Modified catalyst</term><term>Oxidation</term><term>Secondary alcohol</term><term>Supported catalyst</term><term>Titanium Oxides</term></keywords><keywords scheme="Pascal" xml:lang="fr"><term>Etude expérimentale</term><term>Catalyseur sur support</term><term>Catalyseur modifié</term><term>Cobalt</term><term>Titane Oxyde</term><term>Bore</term><term>Réaction catalytique</term><term>Oxydation</term><term>Déshydrogénation</term><term>Ethane</term><term>Alcane</term><term>Hydrocarbure</term><term>Butanol</term><term>Alcool secondaire</term><term>Catalyse hétérogène</term><term>Butan-2-ol</term></keywords><keywords scheme="Wicri" type="topic" xml:lang="fr"><term>Cobalt</term><term>Hydrocarbure</term></keywords></textClass></profileDesc></teiHeader><front><div type="abstract" xml:lang="en">Cobalt- and cobalt-boron-loaded TiO<sub>2</sub> (anatase) catalysts were prepared and characterized before and after catalytic tests by XRD, HRTEM, IR, UV-visible, and laser Raman spectroscopy. Their activity was investigated in oxidative dehydrogenation (ODH) of ethane. In the absence of boron, the best performances were exhibited by the sample containing 7.6 wt% Co, which was selected for further investigations. At 550 °C, it displayed a stationary state with a conversion of 22.2% and an ethylene selectivity around 60%. This catalyst also showed in the first 3 h on stream a 30% decay in activity that was attributed to a concomitant loss of specific surface area and the formation of CoTiO<sub>3</sub> and Co<sub>2</sub>TiO<sub>4</sub> phases. The addition of 0.25 wt% boron to this Co(7.6)/TiO<sub>2</sub> sample improved the ethane conversion and the ethylene selectivity, which attained 28.4 and 67%, respectively. Boron concentrations superior to 0.25 wt% negatively affected the catalysts performances, probably because at high loadings it profoundly modified the acid-base properties of the surface. XRD and HRTEM analyses showed that at the same time the size of Co<sub>3</sub>O<sub>4</sub> crystallites decreased. IR investigations confirmed the increase in acidity upon boron addition and the decrease in strength of the basic sites which were involved in the dehydrogenation processes. The catalytic behavior and the acid-base properties of Co(7.6)/TiO<sub>2</sub> loaded with different amounts of boron were also studied using butan-2-ol conversion. Boron addition enhanced the dehydration and the dehydrogenation reactions. However, above 0.25 wt% it decreased the dehydrogenation activity, confirming the modifications of the properties of the acid-base centers revealed by the IR studies. For this optimal concentration of boron, the activity and the selectivity in butan-2-ol dehydrogenation exhibited a maximum that coincided with the one observed in the ethane ODH, which suggests that both reactions possibly involved the same type of active centers.</div></front></TEI><affiliations><list><country><li>France</li><li>Maroc</li></country><region><li>Rabat-Salé-Kénitra</li><li>Île-de-France</li></region><settlement><li>Paris</li><li>Rabat</li></settlement></list><tree><country name="Maroc"><region name="Rabat-Salé-Kénitra"><name sortKey="Brik, Younes" sort="Brik, Younes" uniqKey="Brik Y" first="Younes" last="Brik">Younes Brik</name></region><name sortKey="Kacimi, Mohamed" sort="Kacimi, Mohamed" uniqKey="Kacimi M" first="Mohamed" last="Kacimi">Mohamed Kacimi</name><name sortKey="Ziyad, Mahfoud" sort="Ziyad, Mahfoud" uniqKey="Ziyad M" first="Mahfoud" last="Ziyad">Mahfoud Ziyad</name></country><country name="France"><region name="Île-de-France"><name sortKey="Brik, Younes" sort="Brik, Younes" uniqKey="Brik Y" first="Younes" last="Brik">Younes Brik</name></region><name sortKey="Bozon Verduraz, Francois" sort="Bozon Verduraz, Francois" uniqKey="Bozon Verduraz F" first="Francois" last="Bozon-Verduraz">Francois Bozon-Verduraz</name></country></tree></affiliations></record>Pour manipuler ce document sous Unix (Dilib)
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