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The activation of NO and CH4 for NO-SCR reaction over In- and Co-containing H-ZSM-5 catalysts

Identifieur interne : 002343 ( Main/Repository ); précédent : 002342; suivant : 002344

The activation of NO and CH4 for NO-SCR reaction over In- and Co-containing H-ZSM-5 catalysts

Auteurs : RBID : Pascal:11-0392019

Descripteurs français

Pascal (Inist)
- Activation, Méthane, Réduction chimique, Spectrométrie IR, Catalyse hétérogène, Monoxyde d'azote, Cobalt, Matériau modifié, Métal transition, Zéolite, Indium, Zéolite ZSM5, Spectrométrie DRIFT, Zéolite HZSM5.
Wicri :
- concept : Cobalt.

English descriptors

KwdEn :
- Activation, Chemical reduction, Cobalt, Heterogeneous catalysis, Indium, Infrared spectrometry, Methane, Modified material, Nitric oxide, Transition metal, Zeolite.

Abstract

The catalytic oxidation of NO to NO₂ (NO-COX) and the selective catalytic reduction of NO to N₂ by methane in the presence of excess oxygen (NO-SCR) was studied over zeolite In,H-, Co,H-, and Co,In,H-ZSM-5 catalysts. The catalysts were characterized by temperature-programmed H₂ reduction (H₂-TPR) and operando DRIFT spectroscopy. The cobalt was present in the catalysts predominantly in Co-oxide clusters, whereas the charge of the zeolite framework was balanced by H⁺ and cationic indium species. The Bronsted acid sites promoted the NO-COX reaction; however, the Co-oxide clusters were much more active in this reaction. In absence of indium the catalysts were inactive in the NO-SCR reaction. The NO/NO₂ mixture formed in the NO-COX reaction was shown to further react with the InO⁺/(InOH)²⁺-zeolite resulting in the simultaneous formation of InNO₃ and NO⁺ species. The Co-oxide clusters increased the rate of NO₂ generation and, thereby, the InNO₃/NO⁺ formation. It was substantiated that an N-containing organic intermediate was obtained in the reaction of methane and nitrate group. Nitrogen was generated in the reaction between the obtained intermediate and the NO⁺. The catalytic cycle must have been closed by the oxidation of In⁺ to InO⁺/(InOH)²⁺ by the reactant mixture.

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Pascal:11-0392019

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<record><TEI><teiHeader><fileDesc><titleStmt><title xml:lang="en" level="a">The activation of NO and CH<sub>4</sub>
 for NO-SCR reaction over In- and Co-containing H-ZSM-5 catalysts</title>
<author><name sortKey="Lonyi, Ferenc" uniqKey="Lonyi F">Ferenc Lonyi</name>
<affiliation wicri:level="1"><inist:fA14 i1="01"><s1>Institute of Nanochemistry and Catalysis, Chemical Research Center, Hungarian Academy of Sciences, Department of Micro- and Mesoporous Materials, Pusztaszeri u. 59-67</s1>
<s2>1025 Budapest</s2>
<s3>HUN</s3>
<sZ>1 aut.</sZ>
<sZ>2 aut.</sZ>
<sZ>3 aut.</sZ>
</inist:fA14>
<country>Hongrie</country>
<placeName><settlement type="city">Budapest</settlement>
<region nuts="2">Hongrie centrale</region>
</placeName>
</affiliation>
</author>
<author><name sortKey="Solt, Hanna E" uniqKey="Solt H">Hanna E. Solt</name>
<affiliation wicri:level="1"><inist:fA14 i1="01"><s1>Institute of Nanochemistry and Catalysis, Chemical Research Center, Hungarian Academy of Sciences, Department of Micro- and Mesoporous Materials, Pusztaszeri u. 59-67</s1>
<s2>1025 Budapest</s2>
<s3>HUN</s3>
<sZ>1 aut.</sZ>
<sZ>2 aut.</sZ>
<sZ>3 aut.</sZ>
</inist:fA14>
<country>Hongrie</country>
<placeName><settlement type="city">Budapest</settlement>
<region nuts="2">Hongrie centrale</region>
</placeName>
</affiliation>
</author>
<author><name sortKey="Valyon, J Zsef" uniqKey="Valyon J">J Zsef Valyon</name>
<affiliation wicri:level="1"><inist:fA14 i1="01"><s1>Institute of Nanochemistry and Catalysis, Chemical Research Center, Hungarian Academy of Sciences, Department of Micro- and Mesoporous Materials, Pusztaszeri u. 59-67</s1>
<s2>1025 Budapest</s2>
<s3>HUN</s3>
<sZ>1 aut.</sZ>
<sZ>2 aut.</sZ>
<sZ>3 aut.</sZ>
</inist:fA14>
<country>Hongrie</country>
<placeName><settlement type="city">Budapest</settlement>
<region nuts="2">Hongrie centrale</region>
</placeName>
</affiliation>
</author>
<author><name sortKey="Boix, Alicia" uniqKey="Boix A">Alicia Boix</name>
<affiliation wicri:level="1"><inist:fA14 i1="02"><s1>Instituto de Investigations en Catálisis y Petroquimica, INCAPE (FIQ, UNL-CONICET), Santiago del Estero 2829</s1>
<s2>3000 Santa Fe</s2>
<s3>ARG</s3>
<sZ>4 aut.</sZ>
<sZ>5 aut.</sZ>
</inist:fA14>
<country>Argentine</country>
<wicri:noRegion>3000 Santa Fe</wicri:noRegion>
</affiliation>
</author>
<author><name sortKey="Gutierrez, Laura B" uniqKey="Gutierrez L">Laura B. Gutierrez</name>
<affiliation wicri:level="1"><inist:fA14 i1="02"><s1>Instituto de Investigations en Catálisis y Petroquimica, INCAPE (FIQ, UNL-CONICET), Santiago del Estero 2829</s1>
<s2>3000 Santa Fe</s2>
<s3>ARG</s3>
<sZ>4 aut.</sZ>
<sZ>5 aut.</sZ>
</inist:fA14>
<country>Argentine</country>
<wicri:noRegion>3000 Santa Fe</wicri:noRegion>
</affiliation>
</author>
</titleStmt>
<publicationStmt><idno type="inist">11-0392019</idno>
<date when="2011">2011</date>
<idno type="stanalyst">PASCAL 11-0392019 INIST</idno>
<idno type="RBID">Pascal:11-0392019</idno>
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<idno type="wicri:Area/Main/Repository">002343</idno>
</publicationStmt>
<seriesStmt><idno type="ISSN">1381-1169</idno>
<title level="j" type="abbreviated">J. mol. catal., A Chem.</title>
<title level="j" type="main">Journal of molecular catalysis. A, Chemical</title>
</seriesStmt>
</fileDesc>
<profileDesc><textClass><keywords scheme="KwdEn" xml:lang="en"><term>Activation</term>
<term>Chemical reduction</term>
<term>Cobalt</term>
<term>Heterogeneous catalysis</term>
<term>Indium</term>
<term>Infrared spectrometry</term>
<term>Methane</term>
<term>Modified material</term>
<term>Nitric oxide</term>
<term>Transition metal</term>
<term>Zeolite</term>
</keywords>
<keywords scheme="Pascal" xml:lang="fr"><term>Activation</term>
<term>Méthane</term>
<term>Réduction chimique</term>
<term>Spectrométrie IR</term>
<term>Catalyse hétérogène</term>
<term>Monoxyde d'azote</term>
<term>Cobalt</term>
<term>Matériau modifié</term>
<term>Métal transition</term>
<term>Zéolite</term>
<term>Indium</term>
<term>Zéolite ZSM5</term>
<term>Spectrométrie DRIFT</term>
<term>Zéolite HZSM5</term>
</keywords>
<keywords scheme="Wicri" type="concept" xml:lang="fr"><term>Cobalt</term>
</keywords>
</textClass>
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<front><div type="abstract" xml:lang="en">The catalytic oxidation of NO to NO<sub>2</sub>
 (NO-COX) and the selective catalytic reduction of NO to N<sub>2</sub>
 by methane in the presence of excess oxygen (NO-SCR) was studied over zeolite In,H-, Co,H-, and Co,In,H-ZSM-5 catalysts. The catalysts were characterized by temperature-programmed H<sub>2</sub>
 reduction (H<sub>2</sub>
-TPR) and operando DRIFT spectroscopy. The cobalt was present in the catalysts predominantly in Co-oxide clusters, whereas the charge of the zeolite framework was balanced by H<sup>+</sup>
 and cationic indium species. The Bronsted acid sites promoted the NO-COX reaction; however, the Co-oxide clusters were much more active in this reaction. In absence of indium the catalysts were inactive in the NO-SCR reaction. The NO/NO<sub>2</sub>
 mixture formed in the NO-COX reaction was shown to further react with the InO<sup>+</sup>
/(InOH)<sup>2+</sup>
-zeolite resulting in the simultaneous formation of InNO<sub>3</sub>
 and NO<sup>+</sup>
 species. The Co-oxide clusters increased the rate of NO<sub>2</sub>
 generation and, thereby, the InNO<sub>3</sub>
/NO<sup>+</sup>
 formation. It was substantiated that an N-containing organic intermediate was obtained in the reaction of methane and nitrate group. Nitrogen was generated in the reaction between the obtained intermediate and the NO<sup>+</sup>
. The catalytic cycle must have been closed by the oxidation of In<sup>+</sup>
 to InO<sup>+</sup>
/(InOH)<sup>2+</sup>
 by the reactant mixture.</div>
</front>
</TEI>
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<fA08 i1="01" i2="1" l="ENG"><s1>The activation of NO and CH<sub>4</sub>
 for NO-SCR reaction over In- and Co-containing H-ZSM-5 catalysts</s1>
</fA08>
<fA11 i1="01" i2="1"><s1>LONYI (Ferenc)</s1>
</fA11>
<fA11 i1="02" i2="1"><s1>SOLT (Hanna E.)</s1>
</fA11>
<fA11 i1="03" i2="1"><s1>VALYON (József)</s1>
</fA11>
<fA11 i1="04" i2="1"><s1>BOIX (Alicia)</s1>
</fA11>
<fA11 i1="05" i2="1"><s1>GUTIERREZ (Laura B.)</s1>
</fA11>
<fA14 i1="01"><s1>Institute of Nanochemistry and Catalysis, Chemical Research Center, Hungarian Academy of Sciences, Department of Micro- and Mesoporous Materials, Pusztaszeri u. 59-67</s1>
<s2>1025 Budapest</s2>
<s3>HUN</s3>
<sZ>1 aut.</sZ>
<sZ>2 aut.</sZ>
<sZ>3 aut.</sZ>
</fA14>
<fA14 i1="02"><s1>Instituto de Investigations en Catálisis y Petroquimica, INCAPE (FIQ, UNL-CONICET), Santiago del Estero 2829</s1>
<s2>3000 Santa Fe</s2>
<s3>ARG</s3>
<sZ>4 aut.</sZ>
<sZ>5 aut.</sZ>
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<fA45><s0>40 ref.</s0>
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<fA47 i1="01" i2="1"><s0>11-0392019</s0>
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</fA66>
<fC01 i1="01" l="ENG"><s0>The catalytic oxidation of NO to NO<sub>2</sub>
 (NO-COX) and the selective catalytic reduction of NO to N<sub>2</sub>
 by methane in the presence of excess oxygen (NO-SCR) was studied over zeolite In,H-, Co,H-, and Co,In,H-ZSM-5 catalysts. The catalysts were characterized by temperature-programmed H<sub>2</sub>
 reduction (H<sub>2</sub>
-TPR) and operando DRIFT spectroscopy. The cobalt was present in the catalysts predominantly in Co-oxide clusters, whereas the charge of the zeolite framework was balanced by H<sup>+</sup>
 and cationic indium species. The Bronsted acid sites promoted the NO-COX reaction; however, the Co-oxide clusters were much more active in this reaction. In absence of indium the catalysts were inactive in the NO-SCR reaction. The NO/NO<sub>2</sub>
 mixture formed in the NO-COX reaction was shown to further react with the InO<sup>+</sup>
/(InOH)<sup>2+</sup>
-zeolite resulting in the simultaneous formation of InNO<sub>3</sub>
 and NO<sup>+</sup>
 species. The Co-oxide clusters increased the rate of NO<sub>2</sub>
 generation and, thereby, the InNO<sub>3</sub>
/NO<sup>+</sup>
 formation. It was substantiated that an N-containing organic intermediate was obtained in the reaction of methane and nitrate group. Nitrogen was generated in the reaction between the obtained intermediate and the NO<sup>+</sup>
. The catalytic cycle must have been closed by the oxidation of In<sup>+</sup>
 to InO<sup>+</sup>
/(InOH)<sup>2+</sup>
 by the reactant mixture.</s0>
</fC01>
<fC02 i1="01" i2="X"><s0>001C01A03</s0>
</fC02>
<fC02 i1="02" i2="X"><s0>001C01I05A</s0>
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<fC03 i1="01" i2="X" l="FRE"><s0>Activation</s0>
<s5>01</s5>
</fC03>
<fC03 i1="01" i2="X" l="ENG"><s0>Activation</s0>
<s5>01</s5>
</fC03>
<fC03 i1="01" i2="X" l="SPA"><s0>Activación</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>Réduction chimique</s0>
<s5>03</s5>
</fC03>
<fC03 i1="03" i2="X" l="ENG"><s0>Chemical reduction</s0>
<s5>03</s5>
</fC03>
<fC03 i1="03" i2="X" l="SPA"><s0>Reducción química</s0>
<s5>03</s5>
</fC03>
<fC03 i1="04" i2="X" l="FRE"><s0>Spectrométrie IR</s0>
<s5>05</s5>
</fC03>
<fC03 i1="04" i2="X" l="ENG"><s0>Infrared spectrometry</s0>
<s5>05</s5>
</fC03>
<fC03 i1="04" i2="X" l="SPA"><s0>Espectrometría IR</s0>
<s5>05</s5>
</fC03>
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<s5>06</s5>
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<s5>06</s5>
</fC03>
<fC03 i1="05" i2="X" l="SPA"><s0>Catálisis heterogénea</s0>
<s5>06</s5>
</fC03>
<fC03 i1="06" i2="X" l="FRE"><s0>Monoxyde d'azote</s0>
<s2>NK</s2>
<s2>FX</s2>
<s5>07</s5>
</fC03>
<fC03 i1="06" i2="X" l="ENG"><s0>Nitric oxide</s0>
<s2>NK</s2>
<s2>FX</s2>
<s5>07</s5>
</fC03>
<fC03 i1="06" i2="X" l="SPA"><s0>Nitrógeno monóxido</s0>
<s2>NK</s2>
<s2>FX</s2>
<s5>07</s5>
</fC03>
<fC03 i1="07" i2="X" l="FRE"><s0>Cobalt</s0>
<s2>NC</s2>
<s5>08</s5>
</fC03>
<fC03 i1="07" i2="X" l="ENG"><s0>Cobalt</s0>
<s2>NC</s2>
<s5>08</s5>
</fC03>
<fC03 i1="07" i2="X" l="SPA"><s0>Cobalto</s0>
<s2>NC</s2>
<s5>08</s5>
</fC03>
<fC03 i1="08" i2="X" l="FRE"><s0>Matériau modifié</s0>
<s5>09</s5>
</fC03>
<fC03 i1="08" i2="X" l="ENG"><s0>Modified material</s0>
<s5>09</s5>
</fC03>
<fC03 i1="08" i2="X" l="SPA"><s0>Material modificado</s0>
<s5>09</s5>
</fC03>
<fC03 i1="09" i2="X" l="FRE"><s0>Métal transition</s0>
<s2>NC</s2>
<s5>10</s5>
</fC03>
<fC03 i1="09" i2="X" l="ENG"><s0>Transition metal</s0>
<s2>NC</s2>
<s5>10</s5>
</fC03>
<fC03 i1="09" i2="X" l="SPA"><s0>Metal transición</s0>
<s2>NC</s2>
<s5>10</s5>
</fC03>
<fC03 i1="10" i2="X" l="FRE"><s0>Zéolite</s0>
<s5>11</s5>
</fC03>
<fC03 i1="10" i2="X" l="ENG"><s0>Zeolite</s0>
<s5>11</s5>
</fC03>
<fC03 i1="10" i2="X" l="SPA"><s0>Zeolita</s0>
<s5>11</s5>
</fC03>
<fC03 i1="11" i2="X" l="FRE"><s0>Indium</s0>
<s2>NC</s2>
<s5>12</s5>
</fC03>
<fC03 i1="11" i2="X" l="ENG"><s0>Indium</s0>
<s2>NC</s2>
<s5>12</s5>
</fC03>
<fC03 i1="11" i2="X" l="SPA"><s0>Indio</s0>
<s2>NC</s2>
<s5>12</s5>
</fC03>
<fC03 i1="12" i2="X" l="FRE"><s0>Zéolite ZSM5</s0>
<s4>INC</s4>
<s5>32</s5>
</fC03>
<fC03 i1="13" i2="X" l="FRE"><s0>Spectrométrie DRIFT</s0>
<s4>INC</s4>
<s5>33</s5>
</fC03>
<fC03 i1="14" i2="X" l="FRE"><s0>Zéolite HZSM5</s0>
<s4>INC</s4>
<s5>34</s5>
</fC03>
<fN21><s1>269</s1>
</fN21>
</pA>
</standard>
</inist>
</record>

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The activation of NO and CH4 for NO-SCR reaction over In- and Co-containing H-ZSM-5 catalysts

The activation of NO and CH4 for NO-SCR reaction over In- and Co-containing H-ZSM-5 catalysts

Descripteurs français

English descriptors

Abstract

Links toward previous steps (curation, corpus...)

Links to Exploration step

Le document en format XML

Pour manipuler ce document sous Unix (Dilib)

Pour mettre un lien sur cette page dans le réseau Wicri