Effect of C3H6 on selective catalytic reduction of NOx by NH3 over a Cu/zeolite catalyst: A mechanistic study

[Display omitted] ▸ C3H6 oxidation intermediates and coke formation induced poisoning, depending on temperature. ▸ Poisoning caused non-monotonic NO changes due to NH3 coverage changes along the catalyst. ▸ Changes in reaction pathways during fast and NO2 SCR in the presence of C3H6 were observed. T...

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Veröffentlicht in:Applied catalysis. B, Environmental Environmental, 2012-07, Vol.123-124, p.296-305
Hauptverfasser: Luo, Jin-Yong, Oh, Harry, Henry, Cary, Epling, William
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container_title Applied catalysis. B, Environmental
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Oh, Harry
Henry, Cary
Epling, William
description [Display omitted] ▸ C3H6 oxidation intermediates and coke formation induced poisoning, depending on temperature. ▸ Poisoning caused non-monotonic NO changes due to NH3 coverage changes along the catalyst. ▸ Changes in reaction pathways during fast and NO2 SCR in the presence of C3H6 were observed. The effects of C3H6 on key SCR reactions over a model Cu/beta zeolite catalyst were characterized using step-response method reactor testing. Under standard SCR conditions, C3H6 clearly inhibited the reduction reaction at 200°C and above. The inhibition was not caused by competitive adsorption between C3H6 and NH3, but by surface intermediate species formed during C3H6 oxidation, including acrolein-like and coke species as indicated by in situ DRIFTS. Similar to the standard SCR reaction, C3H6 also had a negative effect on the fast SCR reaction. Spaci-FTIR (spatially resolved capillary-inlet Fourier transform infrared spectroscopy) results indicated that NO2 was quickly reduced to NO by C3H6, leading to the occurrence of some standard SCR instead of purely fast SCR. However, C3H6 had a positive effect on NO2 SCR. The reduction of NO2 to NO by C3H6 resulted in the occurrence of the fast SCR reaction combined with NO2 SCR instead of pure NO2 SCR. The reaction pathway change also decreased N2O formation significantly.
doi_str_mv 10.1016/j.apcatb.2012.04.038
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B, Environmental</title><description>[Display omitted] ▸ C3H6 oxidation intermediates and coke formation induced poisoning, depending on temperature. ▸ Poisoning caused non-monotonic NO changes due to NH3 coverage changes along the catalyst. ▸ Changes in reaction pathways during fast and NO2 SCR in the presence of C3H6 were observed. The effects of C3H6 on key SCR reactions over a model Cu/beta zeolite catalyst were characterized using step-response method reactor testing. Under standard SCR conditions, C3H6 clearly inhibited the reduction reaction at 200°C and above. The inhibition was not caused by competitive adsorption between C3H6 and NH3, but by surface intermediate species formed during C3H6 oxidation, including acrolein-like and coke species as indicated by in situ DRIFTS. Similar to the standard SCR reaction, C3H6 also had a negative effect on the fast SCR reaction. Spaci-FTIR (spatially resolved capillary-inlet Fourier transform infrared spectroscopy) results indicated that NO2 was quickly reduced to NO by C3H6, leading to the occurrence of some standard SCR instead of purely fast SCR. However, C3H6 had a positive effect on NO2 SCR. The reduction of NO2 to NO by C3H6 resulted in the occurrence of the fast SCR reaction combined with NO2 SCR instead of pure NO2 SCR. The reaction pathway change also decreased N2O formation significantly.</description><subject>Catalyst poisoning</subject><subject>Catalysts</subject><subject>Copper</subject><subject>Diesel emissions</subject><subject>In situ DRIFTS</subject><subject>Nitrogen dioxide</subject><subject>Nitrous oxides</subject><subject>NOx control</subject><subject>Reduction</subject><subject>Selective catalytic reduction</subject><subject>Surface chemistry</subject><subject>Transient-response method</subject><subject>Zeolites</subject><issn>0926-3373</issn><issn>1873-3883</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2012</creationdate><recordtype>article</recordtype><recordid>eNqNkUFr3DAQhUVJoZu0_6AHHXuxM-PxWnIPgbAk3UBILu1ZyNKYavGut5K9ZPvrq2Wba8hp4M33Hsw8Ib4ilAjYXG9Ku3d26soKsCqhLoH0B7FAraggrelCLKCtmoJI0SdxmdIGACqq9EJs7_qe3STHXq5o3chxJxMPWQkHljnTDscpOBnZz1nL2ww-Pb_I7iif1iTHA0dp5Wq-_svjEKZXT5q-y1u5Zffb7kI6JaRp9sfP4mNvh8Rf_s8r8ev-7udqXTw-_3hY3T4WjqCaig6sVb5SChQ7RPTKESE2tgMHNSC12Cwr9J1vubWqd8tOdcuO6lprpT3Qlfh2zt3H8c_MaTLbkBwPg93xOCeDjcJatap5BwpUa0QNy4zWZ9TFMaXIvdnHsLXxmCFzKsJszLkIcyrCQG1yEdl2c7ZxvvgQOJrkAu8c-xDzo40fw9sB_wCik5Fj</recordid><startdate>20120723</startdate><enddate>20120723</enddate><creator>Luo, Jin-Yong</creator><creator>Oh, Harry</creator><creator>Henry, Cary</creator><creator>Epling, William</creator><general>Elsevier B.V</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7ST</scope><scope>C1K</scope><scope>SOI</scope><scope>7SR</scope><scope>7SU</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>FR3</scope><scope>JG9</scope><scope>KR7</scope><scope>L7M</scope></search><sort><creationdate>20120723</creationdate><title>Effect of C3H6 on selective catalytic reduction of NOx by NH3 over a Cu/zeolite catalyst: A mechanistic study</title><author>Luo, Jin-Yong ; Oh, Harry ; Henry, Cary ; Epling, William</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c302t-b0aa7d27707ec111d7c33116ab0c04013916521dbd9e9a7fc5b7b5b3448878d03</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2012</creationdate><topic>Catalyst poisoning</topic><topic>Catalysts</topic><topic>Copper</topic><topic>Diesel emissions</topic><topic>In situ DRIFTS</topic><topic>Nitrogen dioxide</topic><topic>Nitrous oxides</topic><topic>NOx control</topic><topic>Reduction</topic><topic>Selective catalytic reduction</topic><topic>Surface chemistry</topic><topic>Transient-response method</topic><topic>Zeolites</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Luo, Jin-Yong</creatorcontrib><creatorcontrib>Oh, Harry</creatorcontrib><creatorcontrib>Henry, Cary</creatorcontrib><creatorcontrib>Epling, William</creatorcontrib><collection>CrossRef</collection><collection>Environment Abstracts</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Environment Abstracts</collection><collection>Engineered Materials Abstracts</collection><collection>Environmental Engineering Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Engineering Research Database</collection><collection>Materials Research Database</collection><collection>Civil Engineering Abstracts</collection><collection>Advanced Technologies Database with Aerospace</collection><jtitle>Applied catalysis. 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The effects of C3H6 on key SCR reactions over a model Cu/beta zeolite catalyst were characterized using step-response method reactor testing. Under standard SCR conditions, C3H6 clearly inhibited the reduction reaction at 200°C and above. The inhibition was not caused by competitive adsorption between C3H6 and NH3, but by surface intermediate species formed during C3H6 oxidation, including acrolein-like and coke species as indicated by in situ DRIFTS. Similar to the standard SCR reaction, C3H6 also had a negative effect on the fast SCR reaction. Spaci-FTIR (spatially resolved capillary-inlet Fourier transform infrared spectroscopy) results indicated that NO2 was quickly reduced to NO by C3H6, leading to the occurrence of some standard SCR instead of purely fast SCR. However, C3H6 had a positive effect on NO2 SCR. The reduction of NO2 to NO by C3H6 resulted in the occurrence of the fast SCR reaction combined with NO2 SCR instead of pure NO2 SCR. The reaction pathway change also decreased N2O formation significantly.</abstract><pub>Elsevier B.V</pub><doi>10.1016/j.apcatb.2012.04.038</doi><tpages>10</tpages></addata></record>
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subjects Catalyst poisoning
Catalysts
Copper
Diesel emissions
In situ DRIFTS
Nitrogen dioxide
Nitrous oxides
NOx control
Reduction
Selective catalytic reduction
Surface chemistry
Transient-response method
Zeolites
title Effect of C3H6 on selective catalytic reduction of NOx by NH3 over a Cu/zeolite catalyst: A mechanistic study
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