Cobalt-exchanged hydroxyapatite catalysts: Magnetic studies, spectroscopic investigations, performance in 2-butanol and ethane oxidative dehydrogenations
Identifieur interne : 000221 ( France/Analysis ); précédent : 000220; suivant : 000222Cobalt-exchanged hydroxyapatite catalysts: Magnetic studies, spectroscopic investigations, performance in 2-butanol and ethane oxidative dehydrogenations
Auteurs : Kaoutar Elkabouss [Maroc, France] ; Mohamed Kacimi [Maroc] ; Mahfoud Ziyad [Maroc] ; Souad Ammar [France] ; Francois Bozon-Verduraz [France]Source :
- Journal of catalysis : (Print) [ 0021-9517 ] ; 2004.
Descripteurs français
- Pascal (Inist)
- Wicri :
- topic : Cobalt.
English descriptors
- KwdEn :
Abstract
A series of exchanged cobalt/calcium (Co2+/Ca2+) hydroxyapatite Ca10-xCox (PO4)6(OH)2 was synthesized and characterized by XRD, UV-visible-near-infrared (NIR) and IR spectroscopy, magnetic measurements (SQUID), and X-ray photoemission spectroscopy (XPS). The level of Co2+/Ca2+ exchange was limited to 1.35 wt% Co. After calcination in air at 550°C, cobalt was still present as Co2+ and all samples were paramagnetic, showing that the apatite matrix impedes the oxidation of Co2+ and that the Co2+ ions are isolated, whatever the Co content. Magnetic measurements and UV-visible diffuse reflectance spectra show that the exchanged Co2+ ions are hosted by two types of sites (with octahedral and trigonal prismatic symmetries). XPS confirmed the surface cobalt enrichment and did not reveal Co3+ ions. Dehydrogenation of 2-butanol leads almost exclusively to the formation of hutanone. As the Co content increases, the ketone yield passes through a maximum. In the oxidative dehydrogenation of ethane, the ethylene yield also reaches a maximum (22 mol%) for 0.96 wt% Co at 550°C. These results are ascribed to (i) the partial compensation of the intrinsic dehydrogenating activity of cobalt by the decrease in basicity of apatite induced by the replacement of Ca2+ by Co2+, and (ii) the involvement of two types of sites.
Affiliations:
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Pascal:04-0443422Le document en format XML
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<author><name sortKey="Elkabouss, Kaoutar" sort="Elkabouss, Kaoutar" uniqKey="Elkabouss K" first="Kaoutar" last="Elkabouss">Kaoutar Elkabouss</name>
<affiliation wicri:level="3"><inist:fA14 i1="01"><s1>Laboratoire de Physico-Chimie des Matériaux et Catalyse, Faculté des Sciences. Département de Chimie.</s1>
<s2>Rabat</s2>
<s3>MAR</s3>
<sZ>1 aut.</sZ>
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<country>Maroc</country>
<placeName><settlement type="city">Rabat</settlement>
<region nuts="2">Rabat-Salé-Kénitra</region>
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</affiliation>
<affiliation wicri:level="3"><inist:fA14 i1="02"><s1>Groupe de Chimie des Matériaux Divisés et Catalyse, ITODYS, UMR-CNRS 7086, Université Paris 7-Denis Diderot, case 7090, 2, place Jussieu</s1>
<s2>75251 Paris</s2>
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<placeName><region type="region" nuts="2">Île-de-France</region>
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<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>Laboratoire de Physico-Chimie des Matériaux et Catalyse, Faculté des Sciences. Département de Chimie.</s1>
<s2>Rabat</s2>
<s3>MAR</s3>
<sZ>1 aut.</sZ>
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<country>Maroc</country>
<placeName><settlement type="city">Rabat</settlement>
<region nuts="2">Rabat-Salé-Kénitra</region>
</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>Laboratoire de Physico-Chimie des Matériaux et Catalyse, Faculté des Sciences. Département de Chimie.</s1>
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<placeName><settlement type="city">Rabat</settlement>
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</author>
<author><name sortKey="Ammar, Souad" sort="Ammar, Souad" uniqKey="Ammar S" first="Souad" last="Ammar">Souad Ammar</name>
<affiliation wicri:level="3"><inist:fA14 i1="02"><s1>Groupe de Chimie des Matériaux Divisés et Catalyse, ITODYS, UMR-CNRS 7086, Université Paris 7-Denis Diderot, case 7090, 2, place Jussieu</s1>
<s2>75251 Paris</s2>
<s3>FRA</s3>
<sZ>1 aut.</sZ>
<sZ>4 aut.</sZ>
<sZ>5 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="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>Groupe de Chimie des Matériaux Divisés et Catalyse, ITODYS, UMR-CNRS 7086, Université Paris 7-Denis Diderot, case 7090, 2, place Jussieu</s1>
<s2>75251 Paris</s2>
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<sZ>1 aut.</sZ>
<sZ>4 aut.</sZ>
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</inist:fA14>
<country>France</country>
<placeName><region type="region" nuts="2">Île-de-France</region>
<settlement type="city">Paris</settlement>
</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="2004">2004</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>Butanol</term>
<term>Catalyst</term>
<term>Cobalt</term>
<term>Dehydrogenation</term>
<term>Ethane</term>
<term>Hydroxyapatite</term>
<term>Magnetic susceptibility</term>
<term>Oxidation</term>
<term>Photoelectron spectrometry</term>
<term>Reflectance</term>
<term>X ray</term>
</keywords>
<keywords scheme="Pascal" xml:lang="fr"><term>Cobalt</term>
<term>Apatite hydroxylée</term>
<term>Catalyseur</term>
<term>Butanol</term>
<term>Ethane</term>
<term>Oxydation</term>
<term>Déshydrogénation</term>
<term>Facteur réflexion</term>
<term>Susceptibilité magnétique</term>
<term>Spectrométrie photoélectron</term>
<term>Rayon X</term>
</keywords>
<keywords scheme="Wicri" type="topic" xml:lang="fr"><term>Cobalt</term>
</keywords>
</textClass>
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<front><div type="abstract" xml:lang="en">A series of exchanged cobalt/calcium (Co<sup>2+</sup>
/Ca<sup>2+</sup>
) hydroxyapatite Ca<sub>10-x</sub>
Co<sub>x</sub>
(PO<sub>4</sub>
)<sub>6</sub>
(OH)<sub>2</sub>
was synthesized and characterized by XRD, UV-visible-near-infrared (NIR) and IR spectroscopy, magnetic measurements (SQUID), and X-ray photoemission spectroscopy (XPS). The level of Co<sup>2+</sup>
/Ca<sup>2+</sup>
exchange was limited to 1.35 wt% Co. After calcination in air at 550°C, cobalt was still present as Co<sup>2+</sup>
and all samples were paramagnetic, showing that the apatite matrix impedes the oxidation of Co<sup>2+</sup>
and that the Co<sup>2+</sup>
ions are isolated, whatever the Co content. Magnetic measurements and UV-visible diffuse reflectance spectra show that the exchanged Co<sup>2+</sup>
ions are hosted by two types of sites (with octahedral and trigonal prismatic symmetries). XPS confirmed the surface cobalt enrichment and did not reveal Co<sup>3+</sup>
ions. Dehydrogenation of 2-butanol leads almost exclusively to the formation of hutanone. As the Co content increases, the ketone yield passes through a maximum. In the oxidative dehydrogenation of ethane, the ethylene yield also reaches a maximum (22 mol%) for 0.96 wt% Co at 550°C. These results are ascribed to (i) the partial compensation of the intrinsic dehydrogenating activity of cobalt by the decrease in basicity of apatite induced by the replacement of Ca<sup>2+</sup>
by Co<sup>2+</sup>
, and (ii) the involvement of two types of sites.</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="Elkabouss, Kaoutar" sort="Elkabouss, Kaoutar" uniqKey="Elkabouss K" first="Kaoutar" last="Elkabouss">Kaoutar Elkabouss</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="Elkabouss, Kaoutar" sort="Elkabouss, Kaoutar" uniqKey="Elkabouss K" first="Kaoutar" last="Elkabouss">Kaoutar Elkabouss</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="Francois" last="Bozon-Verduraz">Francois Bozon-Verduraz</name>
</country>
</tree>
</affiliations>
</record>
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