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Partial oxidation of methane over modified Keggin-type polyoxotungstates

Identifieur interne : 000020 ( PascalFrancis/Corpus ); précédent : 000019; suivant : 000021

Partial oxidation of methane over modified Keggin-type polyoxotungstates

Auteurs : S. Mansouri ; O. Benlounes ; C. Rabia ; R. Thouvenot ; M. M. Bettahar ; S. Hocine

Source :

RBID : Pascal:13-0358277

Descripteurs français

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.

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Pour connaître la documentation sur le format Inist Standard.

pA  
A01 01  1    @0 1381-1169
A03   1    @0 J. mol. catal., A Chem.
A05       @2 379
A08 01  1  ENG  @1 Partial oxidation of methane over modified Keggin-type polyoxotungstates
A11 01  1    @1 MANSOURI (S.)
A11 02  1    @1 BENLOUNES (O.)
A11 03  1    @1 RABIA (C.)
A11 04  1    @1 THOUVENOT (R.)
A11 05  1    @1 BETTAHAR (M. M.)
A11 06  1    @1 HOCINE (S.)
A14 01      @1 Laboratoire de Chimie Appliquée et de Génie Chimique, Université Mouloud Mammeri - Tizi-Ouzou, BP. 17 R.P @2 1500 Tizi-Ouzou @3 DZA @Z 1 aut. @Z 2 aut. @Z 6 aut.
A14 02      @1 Laboratoire de Chimie du Gaz Naturel, Faculté de Chimie, USTH, B.P 32 @2 El-Alia, Bab-Ezzouar 16111, Alger @3 DZA @Z 3 aut.
A14 03      @1 Institut Parisien de Chimie Moléculaire, UMR 7201, Université Pierre et Marie Curie Equipe Polyoxométallates Case Courier 42,4 Place Jussieu @2 75252 Paris @3 FRA @Z 4 aut.
A14 04      @1 UMR CNRS 7565,IJB, Faculté des Sciences, Nancy Université, Boulevard des Aiguillettes BP 70239 @2 54506 Vandoeuvre-lès-Nancy @3 FRA @Z 5 aut.
A20       @1 255-262
A21       @1 2013
A23 01      @0 ENG
A43 01      @1 INIST @2 17107A @5 354000501074090340
A44       @0 0000 @1 © 2013 INIST-CNRS. All rights reserved.
A45       @0 72 ref.
A47 01  1    @0 13-0358277
A60       @1 P
A61       @0 A
A64 01  1    @0 Journal of molecular catalysis. A, Chemical
A66 01      @0 NLD
C01 01    ENG  @0 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.
C02 01  X    @0 001C01A03
C03 01  X  FRE  @0 Oxydation partielle @5 01
C03 01  X  ENG  @0 Partial oxidation @5 01
C03 01  X  SPA  @0 Oxidación parcial @5 01
C03 02  X  FRE  @0 Méthane @2 NK @2 FX @5 02
C03 02  X  ENG  @0 Methane @2 NK @2 FX @5 02
C03 02  X  SPA  @0 Metano @2 NK @2 FX @5 02
C03 03  X  FRE  @0 Méthanol @2 NK @2 FX @5 03
C03 03  X  ENG  @0 Methanol @2 NK @2 FX @5 03
C03 03  X  SPA  @0 Metanol @2 NK @2 FX @5 03
C03 04  X  FRE  @0 Formaldéhyde @2 NK @2 FX @5 04
C03 04  X  ENG  @0 Formaldehyde @2 NK @2 FX @5 04
C03 04  X  SPA  @0 Formaldehído @2 NK @2 FX @5 04
C03 05  X  FRE  @0 Catalyse hétérogène @5 05
C03 05  X  ENG  @0 Heterogeneous catalysis @5 05
C03 05  X  SPA  @0 Catálisis heterogénea @5 05
C03 06  X  FRE  @0 Polyoxométallate @4 INC @5 32
C07 01  X  FRE  @0 Alcanol @5 06
C07 01  X  ENG  @0 Alkanol @5 06
C07 01  X  SPA  @0 Alcanol @5 06
C07 02  X  FRE  @0 Aldéhyde @5 07
C07 02  X  ENG  @0 Aldehyde @5 07
C07 02  X  SPA  @0 Aldehído @5 07
C07 03  X  FRE  @0 Alcool @5 08
C07 03  X  ENG  @0 Alcohol @5 08
C07 03  X  SPA  @0 Alcohol @5 08
N21       @1 336
N44 01      @1 OTO
N82       @1 OTO

Format Inist (serveur)

NO : PASCAL 13-0358277 INIST
ET : Partial oxidation of methane over modified Keggin-type polyoxotungstates
AU : MANSOURI (S.); BENLOUNES (O.); RABIA (C.); THOUVENOT (R.); BETTAHAR (M. M.); HOCINE (S.)
AF : Laboratoire de Chimie Appliquée et de Génie Chimique, Université Mouloud Mammeri - Tizi-Ouzou, BP. 17 R.P/1500 Tizi-Ouzou/Algérie (1 aut., 2 aut., 6 aut.); Laboratoire de Chimie du Gaz Naturel, Faculté de Chimie, USTH, B.P 32/El-Alia, Bab-Ezzouar 16111, Alger/Algérie (3 aut.); Institut Parisien de Chimie Moléculaire, UMR 7201, Université Pierre et Marie Curie Equipe Polyoxométallates Case Courier 42,4 Place Jussieu/75252 Paris/France (4 aut.); UMR CNRS 7565,IJB, Faculté des Sciences, Nancy Université, Boulevard des Aiguillettes BP 70239/54506 Vandoeuvre-lès-Nancy/France (5 aut.)
DT : Publication en série; Niveau analytique
SO : Journal of molecular catalysis. A, Chemical; ISSN 1381-1169; Pays-Bas; Da. 2013; Vol. 379; Pp. 255-262; Bibl. 72 ref.
LA : Anglais
EA : 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.
CC : 001C01A03
FD : Oxydation partielle; Méthane; Méthanol; Formaldéhyde; Catalyse hétérogène; Polyoxométallate
FG : Alcanol; Aldéhyde; Alcool
ED : Partial oxidation; Methane; Methanol; Formaldehyde; Heterogeneous catalysis
EG : Alkanol; Aldehyde; Alcohol
SD : Oxidación parcial; Metano; Metanol; Formaldehído; Catálisis heterogénea
LO : INIST-17107A.354000501074090340
ID : 13-0358277

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Pascal:13-0358277

Le document en format XML

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<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>
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<s0>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.</s0>
</fC01>
<fC02 i1="01" i2="X">
<s0>001C01A03</s0>
</fC02>
<fC03 i1="01" i2="X" l="FRE">
<s0>Oxydation partielle</s0>
<s5>01</s5>
</fC03>
<fC03 i1="01" i2="X" l="ENG">
<s0>Partial oxidation</s0>
<s5>01</s5>
</fC03>
<fC03 i1="01" i2="X" l="SPA">
<s0>Oxidación parcial</s0>
<s5>01</s5>
</fC03>
<fC03 i1="02" i2="X" l="FRE">
<s0>Méthane</s0>
<s2>NK</s2>
<s2>FX</s2>
<s5>02</s5>
</fC03>
<fC03 i1="02" i2="X" l="ENG">
<s0>Methane</s0>
<s2>NK</s2>
<s2>FX</s2>
<s5>02</s5>
</fC03>
<fC03 i1="02" i2="X" l="SPA">
<s0>Metano</s0>
<s2>NK</s2>
<s2>FX</s2>
<s5>02</s5>
</fC03>
<fC03 i1="03" i2="X" l="FRE">
<s0>Méthanol</s0>
<s2>NK</s2>
<s2>FX</s2>
<s5>03</s5>
</fC03>
<fC03 i1="03" i2="X" l="ENG">
<s0>Methanol</s0>
<s2>NK</s2>
<s2>FX</s2>
<s5>03</s5>
</fC03>
<fC03 i1="03" i2="X" l="SPA">
<s0>Metanol</s0>
<s2>NK</s2>
<s2>FX</s2>
<s5>03</s5>
</fC03>
<fC03 i1="04" i2="X" l="FRE">
<s0>Formaldéhyde</s0>
<s2>NK</s2>
<s2>FX</s2>
<s5>04</s5>
</fC03>
<fC03 i1="04" i2="X" l="ENG">
<s0>Formaldehyde</s0>
<s2>NK</s2>
<s2>FX</s2>
<s5>04</s5>
</fC03>
<fC03 i1="04" i2="X" l="SPA">
<s0>Formaldehído</s0>
<s2>NK</s2>
<s2>FX</s2>
<s5>04</s5>
</fC03>
<fC03 i1="05" i2="X" l="FRE">
<s0>Catalyse hétérogène</s0>
<s5>05</s5>
</fC03>
<fC03 i1="05" i2="X" l="ENG">
<s0>Heterogeneous catalysis</s0>
<s5>05</s5>
</fC03>
<fC03 i1="05" i2="X" l="SPA">
<s0>Catálisis heterogénea</s0>
<s5>05</s5>
</fC03>
<fC03 i1="06" i2="X" l="FRE">
<s0>Polyoxométallate</s0>
<s4>INC</s4>
<s5>32</s5>
</fC03>
<fC07 i1="01" i2="X" l="FRE">
<s0>Alcanol</s0>
<s5>06</s5>
</fC07>
<fC07 i1="01" i2="X" l="ENG">
<s0>Alkanol</s0>
<s5>06</s5>
</fC07>
<fC07 i1="01" i2="X" l="SPA">
<s0>Alcanol</s0>
<s5>06</s5>
</fC07>
<fC07 i1="02" i2="X" l="FRE">
<s0>Aldéhyde</s0>
<s5>07</s5>
</fC07>
<fC07 i1="02" i2="X" l="ENG">
<s0>Aldehyde</s0>
<s5>07</s5>
</fC07>
<fC07 i1="02" i2="X" l="SPA">
<s0>Aldehído</s0>
<s5>07</s5>
</fC07>
<fC07 i1="03" i2="X" l="FRE">
<s0>Alcool</s0>
<s5>08</s5>
</fC07>
<fC07 i1="03" i2="X" l="ENG">
<s0>Alcohol</s0>
<s5>08</s5>
</fC07>
<fC07 i1="03" i2="X" l="SPA">
<s0>Alcohol</s0>
<s5>08</s5>
</fC07>
<fN21>
<s1>336</s1>
</fN21>
<fN44 i1="01">
<s1>OTO</s1>
</fN44>
<fN82>
<s1>OTO</s1>
</fN82>
</pA>
</standard>
<server>
<NO>PASCAL 13-0358277 INIST</NO>
<ET>Partial oxidation of methane over modified Keggin-type polyoxotungstates</ET>
<AU>MANSOURI (S.); BENLOUNES (O.); RABIA (C.); THOUVENOT (R.); BETTAHAR (M. M.); HOCINE (S.)</AU>
<AF>Laboratoire de Chimie Appliquée et de Génie Chimique, Université Mouloud Mammeri - Tizi-Ouzou, BP. 17 R.P/1500 Tizi-Ouzou/Algérie (1 aut., 2 aut., 6 aut.); Laboratoire de Chimie du Gaz Naturel, Faculté de Chimie, USTH, B.P 32/El-Alia, Bab-Ezzouar 16111, Alger/Algérie (3 aut.); Institut Parisien de Chimie Moléculaire, UMR 7201, Université Pierre et Marie Curie Equipe Polyoxométallates Case Courier 42,4 Place Jussieu/75252 Paris/France (4 aut.); UMR CNRS 7565,IJB, Faculté des Sciences, Nancy Université, Boulevard des Aiguillettes BP 70239/54506 Vandoeuvre-lès-Nancy/France (5 aut.)</AF>
<DT>Publication en série; Niveau analytique</DT>
<SO>Journal of molecular catalysis. A, Chemical; ISSN 1381-1169; Pays-Bas; Da. 2013; Vol. 379; Pp. 255-262; Bibl. 72 ref.</SO>
<LA>Anglais</LA>
<EA>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.</EA>
<CC>001C01A03</CC>
<FD>Oxydation partielle; Méthane; Méthanol; Formaldéhyde; Catalyse hétérogène; Polyoxométallate</FD>
<FG>Alcanol; Aldéhyde; Alcool</FG>
<ED>Partial oxidation; Methane; Methanol; Formaldehyde; Heterogeneous catalysis</ED>
<EG>Alkanol; Aldehyde; Alcohol</EG>
<SD>Oxidación parcial; Metano; Metanol; Formaldehído; Catálisis heterogénea</SD>
<LO>INIST-17107A.354000501074090340</LO>
<ID>13-0358277</ID>
</server>
</inist>
</record>

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