Cobalt speciation in cobalt oxide-apatite materials: structure–properties relationship in catalytic oxidative dehydrogenation of ethane and butan-2-ol conversion
Identifieur interne : 000844 ( Main/Exploration ); précédent : 000843; suivant : 000845Cobalt speciation in cobalt oxide-apatite materials: structure–properties relationship in catalytic oxidative dehydrogenation of ethane and butan-2-ol conversion
Auteurs : Kaoutar El Kabouss [Maroc, France] ; Mohamed Kacimi [Maroc] ; Mahfoud Ziyad [Maroc] ; Souad Ammar [France] ; Alain Ensuque [France] ; Jean-Yves Piquemal [France] ; François Bozon-Verduraz [France]Source :
- Journal of Materials Chemistry [ 0959-9428 ] ; 2006.
Abstract
Impregnation of calcium hydroxyapatite by a solution of Co(ii) nitrate followed by calcination at 823 K gives rise to various species, depending on the cobalt content. At low cobalt content (0.2 wt%), the cobalt species are isolated six-coordinated Co2+ ions. For Co content ≥0.4 wt%, the presence of tetrahedral Co2+ and octahedral Co3+ species is attested by UV–visible–NIR spectroscopy, magnetic measurements and XPS data. Magnetic data at low temperature suggest the formation of clustered CoxOy entities. For Co content ≥1.7 wt%, Co3O4 nanocrystals are generated, as evidenced by XRD and magnetic measurements. In the presence of oxygen, the butan-2-ol conversion produces only butan-2-one. The most active catalysts are the cobalt poorest samples which contain only isolated Co2+ ions. Oxidative dehydrogenation of ethane gives a similar trend. Upon increasing the cobalt loading above 0.9 wt%, the specific dehydrogenation activity of Co2+ ions decreases because the nature of the sites changes and the basic properties are lowered. Relationships between the nature of the sites and the catalytic performances are proposed.
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DOI: 10.1039/b602514e
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At low cobalt content (0.2 wt%), the cobalt species are isolated six-coordinated Co2+ ions. For Co content ≥0.4 wt%, the presence of tetrahedral Co2+ and octahedral Co3+ species is attested by UV–visible–NIR spectroscopy, magnetic measurements and XPS data. Magnetic data at low temperature suggest the formation of clustered CoxOy entities. For Co content ≥1.7 wt%, Co3O4 nanocrystals are generated, as evidenced by XRD and magnetic measurements. In the presence of oxygen, the butan-2-ol conversion produces only butan-2-one. The most active catalysts are the cobalt poorest samples which contain only isolated Co2+ ions. Oxidative dehydrogenation of ethane gives a similar trend. Upon increasing the cobalt loading above 0.9 wt%, the specific dehydrogenation activity of Co2+ ions decreases because the nature of the sites changes and the basic properties are lowered. Relationships between the nature of the sites and the catalytic performances are proposed.</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="El Kabouss, Kaoutar" sort="El Kabouss, Kaoutar" uniqKey="El Kabouss K" first="Kaoutar" last="El Kabouss">Kaoutar El Kabouss</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="El Kabouss, Kaoutar" sort="El Kabouss, Kaoutar" uniqKey="El Kabouss K" first="Kaoutar" last="El Kabouss">Kaoutar El Kabouss</name></region><name sortKey="Ammar, Souad" sort="Ammar, Souad" uniqKey="Ammar S" first="Souad" last="Ammar">Souad Ammar</name><name sortKey="Bozon Verduraz, Francois" sort="Bozon Verduraz, Francois" uniqKey="Bozon Verduraz F" first="François" last="Bozon-Verduraz">François Bozon-Verduraz</name><name sortKey="Ensuque, Alain" sort="Ensuque, Alain" uniqKey="Ensuque A" first="Alain" last="Ensuque">Alain Ensuque</name><name sortKey="Piquemal, Jean Yves" sort="Piquemal, Jean Yves" uniqKey="Piquemal J" first="Jean-Yves" last="Piquemal">Jean-Yves Piquemal</name></country></tree></affiliations></record>Pour manipuler ce document sous Unix (Dilib)
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