Relations between structure and catalytic activity of Ce-In-ZSM-5 catalysts for the selective reduction of NO by methane: I. The In-ZSM-5 system
In-ZSM-5 catalysts for the selective catalytic reduction (SCR) of NO by methane have been prepared by different routes (aqueous ion exchange at different pH values; solid-state ion exchange, sublimation, and transport reaction, with an InCl 3 indium source) and compared with respect to their catalyt...
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description | In-ZSM-5 catalysts for the selective catalytic reduction (SCR) of NO by methane have been prepared by different routes (aqueous ion exchange at different pH values; solid-state ion exchange, sublimation, and transport reaction, with an InCl
3 indium source) and compared with respect to their catalytic behavior in the SCR (1000 ppm NO, 1000 ppm methane, 2% O
2 in He, at 30,000 h
−1) to elucidate the origin of differing NO conversion-temperature characteristics observed with the In-ZSM-5 catalyst system. The samples were categorized into those containing intrazeolite indium oxo species exclusively or coexisting with extrazeolite indium oxo aggregates, and materials containing exclusively intrazeolite InO
x
Cl
y
species on the basis of structural information available from EXAFS and XPS studies. In addition, physical mixtures of In(OH)
3 and NH
4-ZSM-5 were studied. The results confirm that intrazeolite indium oxo species are active SCR sites. Their catalytic properties depend on details of the coordination environment. The presence of extrazeolite InO
x
species is hardly reflected in the SCR activity but induces unselective methane activation. The complete failure of an In-silicalite-1 catalyst in NO reduction despite considerable methane activation capability indicates a crucial role of Brønsted acidity for the SCR over In-ZSM-5 catalysts. Intrazeolite InO
x
Cl
y
species exhibit low NO reduction activity, but are able to activate methane as well. With physical mixtures of In
2O
3 and H-ZSM-5 (ex In(OH)
3/NH
4-ZSM-5) activities comparable to those of In-ZSM-5 prepared by aqueous techniques were measured. These activities were obtained only when the constituents were well mixed in the catalyst pellets, while segregation in separate pellets strongly decreased the NO conversions. |
doi_str_mv | 10.1016/S0021-9517(02)00076-3 |
format | Article |
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3 indium source) and compared with respect to their catalytic behavior in the SCR (1000 ppm NO, 1000 ppm methane, 2% O
2 in He, at 30,000 h
−1) to elucidate the origin of differing NO conversion-temperature characteristics observed with the In-ZSM-5 catalyst system. The samples were categorized into those containing intrazeolite indium oxo species exclusively or coexisting with extrazeolite indium oxo aggregates, and materials containing exclusively intrazeolite InO
x
Cl
y
species on the basis of structural information available from EXAFS and XPS studies. In addition, physical mixtures of In(OH)
3 and NH
4-ZSM-5 were studied. The results confirm that intrazeolite indium oxo species are active SCR sites. Their catalytic properties depend on details of the coordination environment. The presence of extrazeolite InO
x
species is hardly reflected in the SCR activity but induces unselective methane activation. The complete failure of an In-silicalite-1 catalyst in NO reduction despite considerable methane activation capability indicates a crucial role of Brønsted acidity for the SCR over In-ZSM-5 catalysts. Intrazeolite InO
x
Cl
y
species exhibit low NO reduction activity, but are able to activate methane as well. With physical mixtures of In
2O
3 and H-ZSM-5 (ex In(OH)
3/NH
4-ZSM-5) activities comparable to those of In-ZSM-5 prepared by aqueous techniques were measured. These activities were obtained only when the constituents were well mixed in the catalyst pellets, while segregation in separate pellets strongly decreased the NO conversions.</description><identifier>ISSN: 0021-9517</identifier><identifier>EISSN: 1090-2694</identifier><identifier>DOI: 10.1016/S0021-9517(02)00076-3</identifier><identifier>CODEN: JCTLA5</identifier><language>eng</language><publisher>Amsterdam: Elsevier Inc</publisher><subject>Active sites ; Catalysis ; Catalysts: preparations and properties ; Chemistry ; Exact sciences and technology ; General and physical chemistry ; In-ZSM-5 ; Ion-exchange ; Methane ; SCR ; Surface physical chemistry ; Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry ; Zeolites: preparations and properties</subject><ispartof>Journal of catalysis, 2003-02, Vol.214 (1), p.100-112</ispartof><rights>2003 Elsevier Science (USA)</rights><rights>2003 INIST-CNRS</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://dx.doi.org/10.1016/S0021-9517(02)00076-3$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>314,780,784,3550,27924,27925,45995</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=14732086$$DView record in Pascal Francis$$Hfree_for_read</backlink></links><search><creatorcontrib>Sowade, T.</creatorcontrib><creatorcontrib>Schmidt, C.</creatorcontrib><creatorcontrib>Schütze, F.-W.</creatorcontrib><creatorcontrib>Berndt, H.</creatorcontrib><creatorcontrib>Grünert, W.</creatorcontrib><title>Relations between structure and catalytic activity of Ce-In-ZSM-5 catalysts for the selective reduction of NO by methane: I. The In-ZSM-5 system</title><title>Journal of catalysis</title><description>In-ZSM-5 catalysts for the selective catalytic reduction (SCR) of NO by methane have been prepared by different routes (aqueous ion exchange at different pH values; solid-state ion exchange, sublimation, and transport reaction, with an InCl
3 indium source) and compared with respect to their catalytic behavior in the SCR (1000 ppm NO, 1000 ppm methane, 2% O
2 in He, at 30,000 h
−1) to elucidate the origin of differing NO conversion-temperature characteristics observed with the In-ZSM-5 catalyst system. The samples were categorized into those containing intrazeolite indium oxo species exclusively or coexisting with extrazeolite indium oxo aggregates, and materials containing exclusively intrazeolite InO
x
Cl
y
species on the basis of structural information available from EXAFS and XPS studies. In addition, physical mixtures of In(OH)
3 and NH
4-ZSM-5 were studied. The results confirm that intrazeolite indium oxo species are active SCR sites. Their catalytic properties depend on details of the coordination environment. The presence of extrazeolite InO
x
species is hardly reflected in the SCR activity but induces unselective methane activation. The complete failure of an In-silicalite-1 catalyst in NO reduction despite considerable methane activation capability indicates a crucial role of Brønsted acidity for the SCR over In-ZSM-5 catalysts. Intrazeolite InO
x
Cl
y
species exhibit low NO reduction activity, but are able to activate methane as well. With physical mixtures of In
2O
3 and H-ZSM-5 (ex In(OH)
3/NH
4-ZSM-5) activities comparable to those of In-ZSM-5 prepared by aqueous techniques were measured. These activities were obtained only when the constituents were well mixed in the catalyst pellets, while segregation in separate pellets strongly decreased the NO conversions.</description><subject>Active sites</subject><subject>Catalysis</subject><subject>Catalysts: preparations and properties</subject><subject>Chemistry</subject><subject>Exact sciences and technology</subject><subject>General and physical chemistry</subject><subject>In-ZSM-5</subject><subject>Ion-exchange</subject><subject>Methane</subject><subject>SCR</subject><subject>Surface physical chemistry</subject><subject>Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry</subject><subject>Zeolites: preparations and properties</subject><issn>0021-9517</issn><issn>1090-2694</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2003</creationdate><recordtype>article</recordtype><recordid>eNo9kU1LAzEQhoMoWKs_QchF0EN0stmkWS8ixY9CteDHxUtIk1mMbLeSpJX9F_5kt1o8zeWZh3nnJeSYwzkHri6eAQrOKslHp1CcAcBIMbFDBhwqYIWqyl0y-Ef2yUFKHwCcS6kH5PsJG5vDsk10jvkLsaUpx5XLq4jUtp46m23T5eCodTmsQ-7osqZjZJOWvT0_MLklUk60Xkaa35EmbHADI43oe1ev3yw9zui8owvM77bFSzo5py89_O9JvQMXh2Svtk3Co-0cktfbm5fxPZvO7ibj6ynDQlSZKa3BK19j4edz56woK1dJ610tldCSl1qKqiz7mIpz0KAsSl5Y7bWrUdVeDMnJn_fTJmebOtrWhWQ-Y1jY2BlejkQBWvXc1R-H_THrgNEkF7B16EPsQxq_DIaD2RRhfoswmy8bKMxvEUaIH52ZfHA</recordid><startdate>20030215</startdate><enddate>20030215</enddate><creator>Sowade, T.</creator><creator>Schmidt, C.</creator><creator>Schütze, F.-W.</creator><creator>Berndt, H.</creator><creator>Grünert, W.</creator><general>Elsevier Inc</general><general>Elsevier</general><scope>IQODW</scope></search><sort><creationdate>20030215</creationdate><title>Relations between structure and catalytic activity of Ce-In-ZSM-5 catalysts for the selective reduction of NO by methane: I. The In-ZSM-5 system</title><author>Sowade, T. ; Schmidt, C. ; Schütze, F.-W. ; Berndt, H. ; Grünert, W.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-e239t-6880d6dfe2dbbcca349c95adcf56385148539440116110806ae512a8d8cfe6fd3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2003</creationdate><topic>Active sites</topic><topic>Catalysis</topic><topic>Catalysts: preparations and properties</topic><topic>Chemistry</topic><topic>Exact sciences and technology</topic><topic>General and physical chemistry</topic><topic>In-ZSM-5</topic><topic>Ion-exchange</topic><topic>Methane</topic><topic>SCR</topic><topic>Surface physical chemistry</topic><topic>Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry</topic><topic>Zeolites: preparations and properties</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Sowade, T.</creatorcontrib><creatorcontrib>Schmidt, C.</creatorcontrib><creatorcontrib>Schütze, F.-W.</creatorcontrib><creatorcontrib>Berndt, H.</creatorcontrib><creatorcontrib>Grünert, W.</creatorcontrib><collection>Pascal-Francis</collection><jtitle>Journal of catalysis</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Sowade, T.</au><au>Schmidt, C.</au><au>Schütze, F.-W.</au><au>Berndt, H.</au><au>Grünert, W.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Relations between structure and catalytic activity of Ce-In-ZSM-5 catalysts for the selective reduction of NO by methane: I. The In-ZSM-5 system</atitle><jtitle>Journal of catalysis</jtitle><date>2003-02-15</date><risdate>2003</risdate><volume>214</volume><issue>1</issue><spage>100</spage><epage>112</epage><pages>100-112</pages><issn>0021-9517</issn><eissn>1090-2694</eissn><coden>JCTLA5</coden><abstract>In-ZSM-5 catalysts for the selective catalytic reduction (SCR) of NO by methane have been prepared by different routes (aqueous ion exchange at different pH values; solid-state ion exchange, sublimation, and transport reaction, with an InCl
3 indium source) and compared with respect to their catalytic behavior in the SCR (1000 ppm NO, 1000 ppm methane, 2% O
2 in He, at 30,000 h
−1) to elucidate the origin of differing NO conversion-temperature characteristics observed with the In-ZSM-5 catalyst system. The samples were categorized into those containing intrazeolite indium oxo species exclusively or coexisting with extrazeolite indium oxo aggregates, and materials containing exclusively intrazeolite InO
x
Cl
y
species on the basis of structural information available from EXAFS and XPS studies. In addition, physical mixtures of In(OH)
3 and NH
4-ZSM-5 were studied. The results confirm that intrazeolite indium oxo species are active SCR sites. Their catalytic properties depend on details of the coordination environment. The presence of extrazeolite InO
x
species is hardly reflected in the SCR activity but induces unselective methane activation. The complete failure of an In-silicalite-1 catalyst in NO reduction despite considerable methane activation capability indicates a crucial role of Brønsted acidity for the SCR over In-ZSM-5 catalysts. Intrazeolite InO
x
Cl
y
species exhibit low NO reduction activity, but are able to activate methane as well. With physical mixtures of In
2O
3 and H-ZSM-5 (ex In(OH)
3/NH
4-ZSM-5) activities comparable to those of In-ZSM-5 prepared by aqueous techniques were measured. These activities were obtained only when the constituents were well mixed in the catalyst pellets, while segregation in separate pellets strongly decreased the NO conversions.</abstract><cop>Amsterdam</cop><pub>Elsevier Inc</pub><doi>10.1016/S0021-9517(02)00076-3</doi><tpages>13</tpages></addata></record> |
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source | Elsevier ScienceDirect Journals Complete |
subjects | Active sites Catalysis Catalysts: preparations and properties Chemistry Exact sciences and technology General and physical chemistry In-ZSM-5 Ion-exchange Methane SCR Surface physical chemistry Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry Zeolites: preparations and properties |
title | Relations between structure and catalytic activity of Ce-In-ZSM-5 catalysts for the selective reduction of NO by methane: I. The In-ZSM-5 system |
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