Kinetic Reaction Models for the Selective Reduction of NO by Methane over Multifunctional Zeolite-based Redox Catalysts
Kinetic measurements of the selective catalytic reduction (SCR) of NO by methane were performed over CeO2/H‐ZSM‐5, In‐ZSM‐5, and CeO2/In‐ZSM‐5 catalysts. The parameter space covered NO, CH4, and O2 concentrations varying from 250 to 1000 ppm, from 500 to 2000 ppm, and from 0.5 to 10 vol.‐%, respecti...
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description | Kinetic measurements of the selective catalytic reduction (SCR) of NO by methane were performed over CeO2/H‐ZSM‐5, In‐ZSM‐5, and CeO2/In‐ZSM‐5 catalysts. The parameter space covered NO, CH4, and O2 concentrations varying from 250 to 1000 ppm, from 500 to 2000 ppm, and from 0.5 to 10 vol.‐%, respectively, space velocities between 5000 and 90000 h–1 and temperatures between 573 and 873 K depending on the catalyst activities. With CeO2/In‐ZSM‐5 an additional series of measurements was performed with moistened feed gas (0.5–10 vol.‐% H2O). On the basis of a pseudo‐homogeneous, one‐dimensional fixed‐bed reactor model, the data were fitted to a kinetic model that includes power rate laws for the reduction of NO and for the unselective total oxidation of methane. From analyses of isothermal data sets, almost all reaction orders were found to vary significantly with changing temperature, which indicates that the simple kinetic model cannot reflect the complex reaction mechanism correctly. Nevertheless, the data measured with In‐ZSM‐5 could be modeled with good accuracy over a wide range of reaction temperatures (150 K) while the accuracy was less satisfactory with the remaining data sets, in particular for data with the moist feed over CeO2/In‐ZSM‐5. With the latter catalyst it was not possible to represent the data measured in dry and in moist feed in a single model even upon confinement to fixed reaction temperatures. A comparison of the separate models established showed strong changes in the reaction orders in the presence of water, which occur apparently already at a very low water content (≤ 0.5 vol.‐%). The kinetic parameters found are in agreement with earlier conclusions about the reaction mechanisms. With In‐ZSM‐5, both reaction orders and the activation energy show a rate‐limiting influence of NO oxidation on the NO reduction path which is removed by the presence of the CeO2 promoter. A difference in the reaction mechanism over CeO2/In‐ZSM‐5 and CeO2/H‐ZSM‐5 is reflected in different kinetic parameters. The differences of the kinetic parameters between dry‐feed and moist‐feed models for CeO2/In‐ZSM‐5 reflect adsorption competition between the reactants and water.
Kinetic measurements of the selective catalytic reduction (SCR) of NO by methane were performed over multifunctional zeolite‐based catalysts. On the basis of a pseudo‐homogeneous, one‐dimensional fixed‐bed reactor model, the data were fitted to a kinetic model that includes power rate laws. The |
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Kinetic measurements of the selective catalytic reduction (SCR) of NO by methane were performed over multifunctional zeolite‐based catalysts. On the basis of a pseudo‐homogeneous, one‐dimensional fixed‐bed reactor model, the data were fitted to a kinetic model that includes power rate laws. The selective catalytic reduction of NO by hydrocarbons (HC‐SCR) has been in the focus of environmental catalysis for many years. The kinetic study of the SCR of NO by methane over a ternary CeO2/In‐ZSM‐5 catalyst and the related CeO2/H‐ZSM‐5 and In‐ZSM‐5 systems, was undertaken to verify the conclusions of an extended investigation of structure and catalytic behavior of CeO2/In‐ZSM‐5 catalysts.</description><identifier>ISSN: 0930-7516</identifier><identifier>EISSN: 1521-4125</identifier><identifier>DOI: 10.1002/ceat.200402132</identifier><identifier>CODEN: CETEER</identifier><language>eng</language><publisher>Weinheim: WILEY-VCH Verlag</publisher><subject>Adsorption ; Applied sciences ; Catalysis ; Catalysts ; Catalytic reactions ; Chemical engineering ; Chemistry ; Exact sciences and technology ; General and physical chemistry ; Kinetics ; Reactors ; Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry ; Zeolites</subject><ispartof>Chemical engineering & technology, 2004-12, Vol.27 (12), p.1277-1289</ispartof><rights>Copyright © 2004 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim</rights><rights>2005 INIST-CNRS</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c3942-a5e330e623de5c2b9c83e3ae43e143a04ba046b633f9f1cc0683fa3f549394263</citedby><cites>FETCH-LOGICAL-c3942-a5e330e623de5c2b9c83e3ae43e143a04ba046b633f9f1cc0683fa3f549394263</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://onlinelibrary.wiley.com/doi/pdf/10.1002%2Fceat.200402132$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fceat.200402132$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>314,780,784,1417,27924,27925,45574,45575</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=16430360$$DView record in Pascal Francis$$Hfree_for_read</backlink></links><search><creatorcontrib>Sowade, T.</creatorcontrib><creatorcontrib>Schütze, F.-W.</creatorcontrib><creatorcontrib>Berndt, H.</creatorcontrib><creatorcontrib>Grünert, W.</creatorcontrib><title>Kinetic Reaction Models for the Selective Reduction of NO by Methane over Multifunctional Zeolite-based Redox Catalysts</title><title>Chemical engineering & technology</title><addtitle>Chem. Eng. Technol</addtitle><description>Kinetic measurements of the selective catalytic reduction (SCR) of NO by methane were performed over CeO2/H‐ZSM‐5, In‐ZSM‐5, and CeO2/In‐ZSM‐5 catalysts. The parameter space covered NO, CH4, and O2 concentrations varying from 250 to 1000 ppm, from 500 to 2000 ppm, and from 0.5 to 10 vol.‐%, respectively, space velocities between 5000 and 90000 h–1 and temperatures between 573 and 873 K depending on the catalyst activities. With CeO2/In‐ZSM‐5 an additional series of measurements was performed with moistened feed gas (0.5–10 vol.‐% H2O). On the basis of a pseudo‐homogeneous, one‐dimensional fixed‐bed reactor model, the data were fitted to a kinetic model that includes power rate laws for the reduction of NO and for the unselective total oxidation of methane. From analyses of isothermal data sets, almost all reaction orders were found to vary significantly with changing temperature, which indicates that the simple kinetic model cannot reflect the complex reaction mechanism correctly. Nevertheless, the data measured with In‐ZSM‐5 could be modeled with good accuracy over a wide range of reaction temperatures (150 K) while the accuracy was less satisfactory with the remaining data sets, in particular for data with the moist feed over CeO2/In‐ZSM‐5. With the latter catalyst it was not possible to represent the data measured in dry and in moist feed in a single model even upon confinement to fixed reaction temperatures. A comparison of the separate models established showed strong changes in the reaction orders in the presence of water, which occur apparently already at a very low water content (≤ 0.5 vol.‐%). The kinetic parameters found are in agreement with earlier conclusions about the reaction mechanisms. With In‐ZSM‐5, both reaction orders and the activation energy show a rate‐limiting influence of NO oxidation on the NO reduction path which is removed by the presence of the CeO2 promoter. A difference in the reaction mechanism over CeO2/In‐ZSM‐5 and CeO2/H‐ZSM‐5 is reflected in different kinetic parameters. The differences of the kinetic parameters between dry‐feed and moist‐feed models for CeO2/In‐ZSM‐5 reflect adsorption competition between the reactants and water.
Kinetic measurements of the selective catalytic reduction (SCR) of NO by methane were performed over multifunctional zeolite‐based catalysts. On the basis of a pseudo‐homogeneous, one‐dimensional fixed‐bed reactor model, the data were fitted to a kinetic model that includes power rate laws. The selective catalytic reduction of NO by hydrocarbons (HC‐SCR) has been in the focus of environmental catalysis for many years. The kinetic study of the SCR of NO by methane over a ternary CeO2/In‐ZSM‐5 catalyst and the related CeO2/H‐ZSM‐5 and In‐ZSM‐5 systems, was undertaken to verify the conclusions of an extended investigation of structure and catalytic behavior of CeO2/In‐ZSM‐5 catalysts.</description><subject>Adsorption</subject><subject>Applied sciences</subject><subject>Catalysis</subject><subject>Catalysts</subject><subject>Catalytic reactions</subject><subject>Chemical engineering</subject><subject>Chemistry</subject><subject>Exact sciences and technology</subject><subject>General and physical chemistry</subject><subject>Kinetics</subject><subject>Reactors</subject><subject>Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry</subject><subject>Zeolites</subject><issn>0930-7516</issn><issn>1521-4125</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2004</creationdate><recordtype>article</recordtype><recordid>eNqFkEFPHDEMRiPUSmwpV8659DhbJ57JMke6AorKgsSCkLhEnqwjQtMZNMkC---Z7VSUGwfLsvyeLX1CHCiYKgD93THlqQYoQSvUO2KiKq2KUunqk5hAjVDMKmV2xZeUHgBADcNEPP8KLefg5BWTy6Fr5aJbcUzSd73M9yyXHHlYPPFArNYj0nl5cSmbjVxwvqeWZffEvVysYw5-3f5lKMo77mLIXDSUeLW1uxc5p0xxk3L6Kj57ion3__U9cXNyfD3_WZxfnp7Nj84Lh3WpC6oYEdhoXHHldFO7Q2QkLpFViQRlM5RpDKKvvXIOzCF6Ql-V9dY3uCem413Xdyn17O1jH_5Qv7EK7DY2u43NvsU2CN9G4ZGSo-h7al1I_y1TIqCBgatH7jlE3nxw1c6Pj67f_yhGN6TML28u9b-tmeGssrcXp1adLH8sb7W2Cl8BqLyOUA</recordid><startdate>200412</startdate><enddate>200412</enddate><creator>Sowade, T.</creator><creator>Schütze, F.-W.</creator><creator>Berndt, H.</creator><creator>Grünert, W.</creator><general>WILEY-VCH Verlag</general><general>WILEY‐VCH Verlag</general><general>Wiley-VCH</general><scope>BSCLL</scope><scope>IQODW</scope><scope>AAYXX</scope><scope>CITATION</scope></search><sort><creationdate>200412</creationdate><title>Kinetic Reaction Models for the Selective Reduction of NO by Methane over Multifunctional Zeolite-based Redox Catalysts</title><author>Sowade, T. ; Schütze, F.-W. ; Berndt, H. ; Grünert, W.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c3942-a5e330e623de5c2b9c83e3ae43e143a04ba046b633f9f1cc0683fa3f549394263</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2004</creationdate><topic>Adsorption</topic><topic>Applied sciences</topic><topic>Catalysis</topic><topic>Catalysts</topic><topic>Catalytic reactions</topic><topic>Chemical engineering</topic><topic>Chemistry</topic><topic>Exact sciences and technology</topic><topic>General and physical chemistry</topic><topic>Kinetics</topic><topic>Reactors</topic><topic>Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry</topic><topic>Zeolites</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Sowade, T.</creatorcontrib><creatorcontrib>Schütze, F.-W.</creatorcontrib><creatorcontrib>Berndt, H.</creatorcontrib><creatorcontrib>Grünert, W.</creatorcontrib><collection>Istex</collection><collection>Pascal-Francis</collection><collection>CrossRef</collection><jtitle>Chemical engineering & technology</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Sowade, T.</au><au>Schütze, F.-W.</au><au>Berndt, H.</au><au>Grünert, W.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Kinetic Reaction Models for the Selective Reduction of NO by Methane over Multifunctional Zeolite-based Redox Catalysts</atitle><jtitle>Chemical engineering & technology</jtitle><addtitle>Chem. Eng. Technol</addtitle><date>2004-12</date><risdate>2004</risdate><volume>27</volume><issue>12</issue><spage>1277</spage><epage>1289</epage><pages>1277-1289</pages><issn>0930-7516</issn><eissn>1521-4125</eissn><coden>CETEER</coden><abstract>Kinetic measurements of the selective catalytic reduction (SCR) of NO by methane were performed over CeO2/H‐ZSM‐5, In‐ZSM‐5, and CeO2/In‐ZSM‐5 catalysts. The parameter space covered NO, CH4, and O2 concentrations varying from 250 to 1000 ppm, from 500 to 2000 ppm, and from 0.5 to 10 vol.‐%, respectively, space velocities between 5000 and 90000 h–1 and temperatures between 573 and 873 K depending on the catalyst activities. With CeO2/In‐ZSM‐5 an additional series of measurements was performed with moistened feed gas (0.5–10 vol.‐% H2O). On the basis of a pseudo‐homogeneous, one‐dimensional fixed‐bed reactor model, the data were fitted to a kinetic model that includes power rate laws for the reduction of NO and for the unselective total oxidation of methane. From analyses of isothermal data sets, almost all reaction orders were found to vary significantly with changing temperature, which indicates that the simple kinetic model cannot reflect the complex reaction mechanism correctly. Nevertheless, the data measured with In‐ZSM‐5 could be modeled with good accuracy over a wide range of reaction temperatures (150 K) while the accuracy was less satisfactory with the remaining data sets, in particular for data with the moist feed over CeO2/In‐ZSM‐5. With the latter catalyst it was not possible to represent the data measured in dry and in moist feed in a single model even upon confinement to fixed reaction temperatures. A comparison of the separate models established showed strong changes in the reaction orders in the presence of water, which occur apparently already at a very low water content (≤ 0.5 vol.‐%). The kinetic parameters found are in agreement with earlier conclusions about the reaction mechanisms. With In‐ZSM‐5, both reaction orders and the activation energy show a rate‐limiting influence of NO oxidation on the NO reduction path which is removed by the presence of the CeO2 promoter. A difference in the reaction mechanism over CeO2/In‐ZSM‐5 and CeO2/H‐ZSM‐5 is reflected in different kinetic parameters. The differences of the kinetic parameters between dry‐feed and moist‐feed models for CeO2/In‐ZSM‐5 reflect adsorption competition between the reactants and water.
Kinetic measurements of the selective catalytic reduction (SCR) of NO by methane were performed over multifunctional zeolite‐based catalysts. On the basis of a pseudo‐homogeneous, one‐dimensional fixed‐bed reactor model, the data were fitted to a kinetic model that includes power rate laws. The selective catalytic reduction of NO by hydrocarbons (HC‐SCR) has been in the focus of environmental catalysis for many years. The kinetic study of the SCR of NO by methane over a ternary CeO2/In‐ZSM‐5 catalyst and the related CeO2/H‐ZSM‐5 and In‐ZSM‐5 systems, was undertaken to verify the conclusions of an extended investigation of structure and catalytic behavior of CeO2/In‐ZSM‐5 catalysts.</abstract><cop>Weinheim</cop><pub>WILEY-VCH Verlag</pub><doi>10.1002/ceat.200402132</doi><tpages>13</tpages></addata></record> |
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subjects | Adsorption Applied sciences Catalysis Catalysts Catalytic reactions Chemical engineering Chemistry Exact sciences and technology General and physical chemistry Kinetics Reactors Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry Zeolites |
title | Kinetic Reaction Models for the Selective Reduction of NO by Methane over Multifunctional Zeolite-based Redox Catalysts |
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