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Oxidative dehydrogenation of ethane and propane over magnesium-cobalt phosphates CoxMg3-x(PO4)2

Identifieur interne : 000143 ( Maroc/Analysis ); précédent : 000142; suivant : 000144

Oxidative dehydrogenation of ethane and propane over magnesium-cobalt phosphates CoxMg3-x(PO4)2

Auteurs : Abdellah Aaddane [Maroc] ; Mohamed Kacimi [Maroc] ; Mahfoud Ziyad [Maroc]

Source :

RBID : Pascal:01-0323119

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English descriptors

Abstract

The magnesium-cobalt phosphates CoxMg3-x(PO4)2 belonging to the olivine-type structure were synthesized by coprecipitation and then investigated in the oxidative dehydrogenation (ODH) of ethane and propane. The best yields, with the exception of Co0.5Mg2.5(PO4)2, were achieved with the compositions ranging between 1 ≤ x ≤ 2.5. Magnesium phosphate Mg3(PO4)2 displayed no activity and pure cobalt phosphate Co3(PO4)2 was found to be the less active component of the solid solution. Comparison of the catalysts performances showed that they all have similar activity in ethane and propane ODH, albeit, they are more selective in propylene than in ethylene production. The CoxMg3-x(PO4)2 solid solution was also studied, for characterization purposes, in butan-2-ol conversion. The samples presented acid-base properties due essentially to the (PO-H) groups but they do not bear conventional redox centers. All the catalysts were active at low temperatures in the alcohol dehydration. The dehydrogenation activity versus the phosphates composition displayed two maxima around x = I and 2, respectively. Similar striking behavior was also observed in ethane and propane ODH. UV-visible investigations of CoxMg3-x(PO4)2 showed, in agreement with the XRD data, that the Co2+ ions are distributed in the phosphate framework between six-and five-coordinated sites. The cobalt atoms in the five-coordinated sites Co(5) and their Co(5)-Co(5) interatomic distances were assumed to play the main role in the C-H bond activation and the appearance of maxima in the activity. Magnesium cations presumably intervene in acid-base properties of the samples and O2 activation. Characterization of the samples showed that they do not undergo any noticeable transformation after the catalytic tests.


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Pascal:01-0323119

Le document en format XML

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<title xml:lang="en" level="a">Oxidative dehydrogenation of ethane and propane over magnesium-cobalt phosphates Co
<sub>x</sub>
Mg
<sub>3-x</sub>
(PO
<sub>4</sub>
)
<sub>2</sub>
</title>
<author>
<name sortKey="Aaddane, Abdellah" sort="Aaddane, Abdellah" uniqKey="Aaddane A" first="Abdellah" last="Aaddane">Abdellah Aaddane</name>
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<s1>Faculté des Sciences, Département de Chimie, Laboratoire de Physico-Chimie des Matériaux et Catalyse, Avenue Ibn Batouta, BP 1014</s1>
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<country>Maroc</country>
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<name sortKey="Kacimi, Mohamed" sort="Kacimi, Mohamed" uniqKey="Kacimi M" first="Mohamed" last="Kacimi">Mohamed Kacimi</name>
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<title xml:lang="en" level="a">Oxidative dehydrogenation of ethane and propane over magnesium-cobalt phosphates Co
<sub>x</sub>
Mg
<sub>3-x</sub>
(PO
<sub>4</sub>
)
<sub>2</sub>
</title>
<author>
<name sortKey="Aaddane, Abdellah" sort="Aaddane, Abdellah" uniqKey="Aaddane A" first="Abdellah" last="Aaddane">Abdellah Aaddane</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 Batouta, BP 1014</s1>
<s2>Rabat</s2>
<s3>MAR</s3>
<sZ>1 aut.</sZ>
<sZ>2 aut.</sZ>
<sZ>3 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="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 Batouta, BP 1014</s1>
<s2>Rabat</s2>
<s3>MAR</s3>
<sZ>1 aut.</sZ>
<sZ>2 aut.</sZ>
<sZ>3 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="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 Batouta, BP 1014</s1>
<s2>Rabat</s2>
<s3>MAR</s3>
<sZ>1 aut.</sZ>
<sZ>2 aut.</sZ>
<sZ>3 aut.</sZ>
</inist:fA14>
<country>Maroc</country>
<placeName>
<settlement type="city">Rabat</settlement>
<region nuts="2">Rabat-Salé-Kénitra</region>
</placeName>
</affiliation>
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<series>
<title level="j" type="main">Catalysis letters</title>
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<keywords scheme="KwdEn" xml:lang="en">
<term>Alkane</term>
<term>Catalyst</term>
<term>Catalytic reaction</term>
<term>Cobalt Phosphates</term>
<term>Dehydrogenation</term>
<term>Ethane</term>
<term>Heterogeneous catalysis</term>
<term>Hydrocarbon</term>
<term>Magnesium phosphate</term>
<term>Oxidation</term>
<term>Propane</term>
<term>Quaternary compound</term>
<term>Solid solution</term>
</keywords>
<keywords scheme="Pascal" xml:lang="fr">
<term>Déshydrogénation</term>
<term>Ethane</term>
<term>Propane</term>
<term>Magnésium phosphate</term>
<term>Cobalt Phosphate</term>
<term>Réaction catalytique</term>
<term>Composé quaternaire</term>
<term>Hydrocarbure</term>
<term>Alcane</term>
<term>Oxydation</term>
<term>Solution solide</term>
<term>Catalyse hétérogène</term>
<term>Catalyseur</term>
<term>CoxMg3-x(PO4)2</term>
<term>Co Mg O P</term>
</keywords>
<keywords scheme="Wicri" type="topic" xml:lang="fr">
<term>Propane</term>
<term>Hydrocarbure</term>
</keywords>
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<front>
<div type="abstract" xml:lang="en">The magnesium-cobalt phosphates Co
<sub>x</sub>
Mg
<sub>3-x</sub>
(PO
<sub>4</sub>
)
<sub>2</sub>
belonging to the olivine-type structure were synthesized by coprecipitation and then investigated in the oxidative dehydrogenation (ODH) of ethane and propane. The best yields, with the exception of Co
<sub>0.5</sub>
Mg
<sub>2.5</sub>
(PO
<sub>4</sub>
)
<sub>2</sub>
, were achieved with the compositions ranging between 1 ≤ x ≤ 2.5. Magnesium phosphate Mg
<sub>3</sub>
(PO
<sub>4</sub>
)
<sub>2</sub>
displayed no activity and pure cobalt phosphate Co
<sub>3</sub>
(PO
<sub>4</sub>
)
<sub>2</sub>
was found to be the less active component of the solid solution. Comparison of the catalysts performances showed that they all have similar activity in ethane and propane ODH, albeit, they are more selective in propylene than in ethylene production. The Co
<sub>x</sub>
Mg
<sub>3-x</sub>
(PO
<sub>4</sub>
)
<sub>2</sub>
solid solution was also studied, for characterization purposes, in butan-2-ol conversion. The samples presented acid-base properties due essentially to the (PO-H) groups but they do not bear conventional redox centers. All the catalysts were active at low temperatures in the alcohol dehydration. The dehydrogenation activity versus the phosphates composition displayed two maxima around x = I and 2, respectively. Similar striking behavior was also observed in ethane and propane ODH. UV-visible investigations of Co
<sub>x</sub>
Mg
<sub>3-x</sub>
(PO
<sub>4</sub>
)
<sub>2</sub>
showed, in agreement with the XRD data, that the Co
<sup>2+</sup>
ions are distributed in the phosphate framework between six-and five-coordinated sites. The cobalt atoms in the five-coordinated sites Co(5) and their Co(5)-Co(5) interatomic distances were assumed to play the main role in the C-H bond activation and the appearance of maxima in the activity. Magnesium cations presumably intervene in acid-base properties of the samples and O
<sub>2</sub>
activation. Characterization of the samples showed that they do not undergo any noticeable transformation after the catalytic tests.</div>
</front>
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<li>Maroc</li>
</country>
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<li>Rabat-Salé-Kénitra</li>
</region>
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<li>Rabat</li>
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<tree>
<country name="Maroc">
<region name="Rabat-Salé-Kénitra">
<name sortKey="Aaddane, Abdellah" sort="Aaddane, Abdellah" uniqKey="Aaddane A" first="Abdellah" last="Aaddane">Abdellah Aaddane</name>
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<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>
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