Partial oxidation of methane over modified Keggin-type polyoxotungstates
Identifieur interne : 000333 ( Main/Exploration ); précédent : 000332; suivant : 000334Partial oxidation of methane over modified Keggin-type polyoxotungstates
Auteurs : S. Mansouri [Algérie] ; O. Benlounes [Algérie] ; C. Rabia [Algérie] ; R. Thouvenot [France] ; M. M. Bettahar [France] ; S. Hocine [Algérie]Source :
- Journal of molecular catalysis. A, Chemical [ 1381-1169 ] ; 2013.
Descripteurs français
- Pascal (Inist)
- Wicri :
- topic : Méthanol.
English descriptors
Abstract
Partial oxidation of methane by molecular oxygen and nitrous oxide was studied in the presence of catalytic amounts of the Keggin-type heteropolyoxometalates of general formula [PW11MO39)(7-n)- with M = Co(II), Ni(II), and Fe(III). The catalysts were prepared by refilling the vacant site of the lacunary precursor K7PW11O39 by the metal additives and characterized by 31P NMR, UV-vis and IR spectra, XRD, TGA/DTA and cyclic voltammetry. The oxidation reaction was performed at atmospheric pressure at 873 or 923 K. Reaction products observed were methanol, formaldehyde, carbon oxides and water. Most prominent results are the following: (i) selectivity to oxygenates as high as 48% (conversion 5%) was obtained; (ii) cobalt and iron doped polyoxometalates were the most active and selective catalysts; (iii) N2O was more reactive and selective than O2. The activity rise was correlated with the increase of the oxidant character of the cluster metal. Kinetic study and catalyst behaviour suggested that reaction paths were different for nitrous oxide and molecular oxygen. For N2O, methane would be oxidized by MO2 centres to methoxy species, precursors of both methanol and formaldehyde. For O2, methane activation rather involves hydrogen abstraction by the lattice oxygen on M = 0 centres to form metal-methyl species, the key-intermediates in the oxidation processes.
Affiliations:
- Algérie, France
- Grand Est, Lorraine (région), Wilaya d'Alger, Île-de-France
- Alger, Paris, Vandoeuvre-lès-Nancy
- Nancy-Université
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Le document en format XML
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Mansouri</name><affiliation wicri:level="1"><inist:fA14 i1="01"><s1>Laboratoire de Chimie Appliquée et de Génie Chimique, Université Mouloud Mammeri - Tizi-Ouzou, BP. 17 R.P</s1><s2>1500 Tizi-Ouzou</s2><s3>DZA</s3><sZ>1 aut.</sZ><sZ>2 aut.</sZ><sZ>6 aut.</sZ></inist:fA14><country>Algérie</country><wicri:noRegion>1500 Tizi-Ouzou</wicri:noRegion></affiliation></author><author><name sortKey="Benlounes, O" sort="Benlounes, O" uniqKey="Benlounes O" first="O." last="Benlounes">O. Benlounes</name><affiliation wicri:level="1"><inist:fA14 i1="01"><s1>Laboratoire de Chimie Appliquée et de Génie Chimique, Université Mouloud Mammeri - Tizi-Ouzou, BP. 17 R.P</s1><s2>1500 Tizi-Ouzou</s2><s3>DZA</s3><sZ>1 aut.</sZ><sZ>2 aut.</sZ><sZ>6 aut.</sZ></inist:fA14><country>Algérie</country><wicri:noRegion>1500 Tizi-Ouzou</wicri:noRegion></affiliation></author><author><name sortKey="Rabia, C" sort="Rabia, C" uniqKey="Rabia C" first="C." last="Rabia">C. Rabia</name><affiliation wicri:level="3"><inist:fA14 i1="02"><s1>Laboratoire de Chimie du Gaz Naturel, Faculté de Chimie, USTH, B.P 32</s1><s2>El-Alia, Bab-Ezzouar 16111, Alger</s2><s3>DZA</s3><sZ>3 aut.</sZ></inist:fA14><country>Algérie</country><placeName><settlement type="city">Alger</settlement><region nuts="2">Wilaya d'Alger</region></placeName></affiliation></author><author><name sortKey="Thouvenot, R" sort="Thouvenot, R" uniqKey="Thouvenot R" first="R." last="Thouvenot">R. Thouvenot</name><affiliation wicri:level="3"><inist:fA14 i1="03"><s1>Institut Parisien de Chimie Moléculaire, UMR 7201, Université Pierre et Marie Curie Equipe Polyoxométallates Case Courier 42,4 Place Jussieu</s1><s2>75252 Paris</s2><s3>FRA</s3><sZ>4 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="Bettahar, M M" sort="Bettahar, M M" uniqKey="Bettahar M" first="M. M." last="Bettahar">M. M. Bettahar</name><affiliation wicri:level="4"><inist:fA14 i1="04"><s1>UMR CNRS 7565,IJB, Faculté des Sciences, Nancy Université, Boulevard des Aiguillettes BP 70239</s1><s2>54506 Vandoeuvre-lès-Nancy</s2><s3>FRA</s3><sZ>5 aut.</sZ></inist:fA14><country>France</country><placeName><region type="region" nuts="2">Grand Est</region><region type="old region" nuts="2">Lorraine (région)</region><settlement type="city">Vandoeuvre-lès-Nancy</settlement></placeName><orgName type="university">Nancy-Université</orgName></affiliation></author><author><name sortKey="Hocine, S" sort="Hocine, S" uniqKey="Hocine S" first="S." last="Hocine">S. Hocine</name><affiliation wicri:level="1"><inist:fA14 i1="01"><s1>Laboratoire de Chimie Appliquée et de Génie Chimique, Université Mouloud Mammeri - Tizi-Ouzou, BP. 17 R.P</s1><s2>1500 Tizi-Ouzou</s2><s3>DZA</s3><sZ>1 aut.</sZ><sZ>2 aut.</sZ><sZ>6 aut.</sZ></inist:fA14><country>Algérie</country><wicri:noRegion>1500 Tizi-Ouzou</wicri:noRegion></affiliation></author></analytic><series><title level="j" type="main">Journal of molecular catalysis. A, Chemical</title><title level="j" type="abbreviated">J. mol. catal., A Chem.</title><idno type="ISSN">1381-1169</idno><imprint><date when="2013">2013</date></imprint></series></biblStruct></sourceDesc><seriesStmt><title level="j" type="main">Journal of molecular catalysis. A, Chemical</title><title level="j" type="abbreviated">J. mol. catal., A Chem.</title><idno type="ISSN">1381-1169</idno></seriesStmt></fileDesc><profileDesc><textClass><keywords scheme="KwdEn" xml:lang="en"><term>Formaldehyde</term><term>Heterogeneous catalysis</term><term>Methane</term><term>Methanol</term><term>Partial oxidation</term></keywords><keywords scheme="Pascal" xml:lang="fr"><term>Oxydation partielle</term><term>Méthane</term><term>Méthanol</term><term>Formaldéhyde</term><term>Catalyse hétérogène</term><term>Polyoxométallate</term></keywords><keywords scheme="Wicri" type="topic" xml:lang="fr"><term>Méthanol</term></keywords></textClass></profileDesc></teiHeader><front><div type="abstract" xml:lang="en">Partial oxidation of methane by molecular oxygen and nitrous oxide was studied in the presence of catalytic amounts of the Keggin-type heteropolyoxometalates of general formula [PW<sub>11</sub>MO<sub>39</sub>)<sup>(7-n)-</sup> with M = Co(II), Ni(II), and Fe(III). The catalysts were prepared by refilling the vacant site of the lacunary precursor K<sub>7</sub>PW<sub>11</sub>O<sub>39</sub> by the metal additives and characterized by <sup>31</sup>P NMR, UV-vis and IR spectra, XRD, TGA/DTA and cyclic voltammetry. The oxidation reaction was performed at atmospheric pressure at 873 or 923 K. Reaction products observed were methanol, formaldehyde, carbon oxides and water. Most prominent results are the following: (i) selectivity to oxygenates as high as 48% (conversion 5%) was obtained; (ii) cobalt and iron doped polyoxometalates were the most active and selective catalysts; (iii) N<sub>2</sub>O was more reactive and selective than O<sub>2</sub>. The activity rise was correlated with the increase of the oxidant character of the cluster metal. Kinetic study and catalyst behaviour suggested that reaction paths were different for nitrous oxide and molecular oxygen. For N<sub>2</sub>O, methane would be oxidized by MO<sub>2</sub> centres to methoxy species, precursors of both methanol and formaldehyde. For O<sub>2</sub>, methane activation rather involves hydrogen abstraction by the lattice oxygen on M = 0 centres to form metal-methyl species, the key-intermediates in the oxidation processes.</div></front></TEI><affiliations><list><country><li>Algérie</li><li>France</li></country><region><li>Grand Est</li><li>Lorraine (région)</li><li>Wilaya d'Alger</li><li>Île-de-France</li></region><settlement><li>Alger</li><li>Paris</li><li>Vandoeuvre-lès-Nancy</li></settlement><orgName><li>Nancy-Université</li></orgName></list><tree><country name="Algérie"><noRegion><name sortKey="Mansouri, S" sort="Mansouri, S" uniqKey="Mansouri S" first="S." last="Mansouri">S. Mansouri</name></noRegion><name sortKey="Benlounes, O" sort="Benlounes, O" uniqKey="Benlounes O" first="O." last="Benlounes">O. Benlounes</name><name sortKey="Hocine, S" sort="Hocine, S" uniqKey="Hocine S" first="S." last="Hocine">S. Hocine</name><name sortKey="Rabia, C" sort="Rabia, C" uniqKey="Rabia C" first="C." last="Rabia">C. Rabia</name></country><country name="France"><region name="Île-de-France"><name sortKey="Thouvenot, R" sort="Thouvenot, R" uniqKey="Thouvenot R" first="R." last="Thouvenot">R. Thouvenot</name></region><name sortKey="Bettahar, M M" sort="Bettahar, M M" uniqKey="Bettahar M" first="M. M." last="Bettahar">M. M. Bettahar</name></country></tree></affiliations></record>Pour manipuler ce document sous Unix (Dilib)
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