Selectivity and Sustainability of a Pd-In/γ-Al₂O₃ Catalyst in a Packed-Bed Reactor: The Effect of Solution Composition
This study tested the selectivity and sustainability of an alumina-supported Pd-In bimetallic catalyst for nitrate reduction with H₂ in a continuous-flow packed-bed reactor in the presence of: (i) dissolved oxygen (DO), an alternative electron acceptor to nitrate, (ii) variable NO₃ ⁻:H₂ influent loa...
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Veröffentlicht in: | Catalysis letters 2009-06, Vol.130 (1-2), p.56-62 |
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description | This study tested the selectivity and sustainability of an alumina-supported Pd-In bimetallic catalyst for nitrate reduction with H₂ in a continuous-flow packed-bed reactor in the presence of: (i) dissolved oxygen (DO), an alternative electron acceptor to nitrate, (ii) variable NO₃ ⁻:H₂ influent loadings, and (iii) the presence of a known foulant, sulfide. The sustainability of the catalyst was promising, as the catalyst was found to be stable under all conditions tested with respect to metal leaching. The presence of DO at concentrations typical of treatment conditions will increase H₂ demand for NO₃ ⁻ reduction, but has no negative impact on the selectivity of the catalyst. Under optimal conditions, i.e., a pH of 5.0 and a high NO₃ ⁻:H₂ influent loading, low NH₃ selectivity (5%) was achieved for extended periods (36 days), resulting in sustained levels of NH₃ that approached the European legal limit. The biggest challenge to the sustainability of the catalyst was the addition of sulfide, that initially increased NH₃ selectivity and ultimately resulted in complete deactivation of the catalyst. Further work is required to identify regeneration methods to restore sulfide-fouled catalyst activity and selectivity; however, the most effective use would be to remove sulfide prior to catalytic treatment. |
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The sustainability of the catalyst was promising, as the catalyst was found to be stable under all conditions tested with respect to metal leaching. The presence of DO at concentrations typical of treatment conditions will increase H₂ demand for NO₃ ⁻ reduction, but has no negative impact on the selectivity of the catalyst. Under optimal conditions, i.e., a pH of 5.0 and a high NO₃ ⁻:H₂ influent loading, low NH₃ selectivity (5%) was achieved for extended periods (36 days), resulting in sustained levels of NH₃ that approached the European legal limit. The biggest challenge to the sustainability of the catalyst was the addition of sulfide, that initially increased NH₃ selectivity and ultimately resulted in complete deactivation of the catalyst. Further work is required to identify regeneration methods to restore sulfide-fouled catalyst activity and selectivity; however, the most effective use would be to remove sulfide prior to catalytic treatment.</description><identifier>ISSN: 1011-372X</identifier><identifier>EISSN: 1572-879X</identifier><identifier>DOI: 10.1007/s10562-009-9883-4</identifier><language>eng</language><publisher>Boston: Boston : Springer US</publisher><subject>Aluminum oxide ; Ammonia ; Bimetals ; Catalysis ; Catalysts ; Chemistry ; Chemistry and Materials Science ; Composition effects ; Deactivation ; Exact sciences and technology ; Fouling ; General and physical chemistry ; Identification methods ; Industrial Chemistry/Chemical Engineering ; Leaching ; Organometallic Chemistry ; Palladium ; Physical Chemistry ; Reduction ; Regeneration ; Selectivity ; Sustainability ; Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry ; Transitional aluminas</subject><ispartof>Catalysis letters, 2009-06, Vol.130 (1-2), p.56-62</ispartof><rights>Springer Science+Business Media, LLC 2009</rights><rights>2009 INIST-CNRS</rights><rights>Catalysis Letters is a copyright of Springer, (2009). All Rights Reserved.</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c300t-6b101d94e817dc96277d980c7c504ef8047c2c71da4b7c4a2efd1167868c3a723</citedby><cites>FETCH-LOGICAL-c300t-6b101d94e817dc96277d980c7c504ef8047c2c71da4b7c4a2efd1167868c3a723</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://link.springer.com/content/pdf/10.1007/s10562-009-9883-4$$EPDF$$P50$$Gspringer$$H</linktopdf><linktohtml>$$Uhttps://link.springer.com/10.1007/s10562-009-9883-4$$EHTML$$P50$$Gspringer$$H</linktohtml><link.rule.ids>314,780,784,27924,27925,41488,42557,51319</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=21698454$$DView record in Pascal Francis$$Hfree_for_read</backlink></links><search><creatorcontrib>Chaplin, Brian P</creatorcontrib><creatorcontrib>Shapley, John R</creatorcontrib><creatorcontrib>Werth, Charles J</creatorcontrib><title>Selectivity and Sustainability of a Pd-In/γ-Al₂O₃ Catalyst in a Packed-Bed Reactor: The Effect of Solution Composition</title><title>Catalysis letters</title><addtitle>Catal Lett</addtitle><description>This study tested the selectivity and sustainability of an alumina-supported Pd-In bimetallic catalyst for nitrate reduction with H₂ in a continuous-flow packed-bed reactor in the presence of: (i) dissolved oxygen (DO), an alternative electron acceptor to nitrate, (ii) variable NO₃ ⁻:H₂ influent loadings, and (iii) the presence of a known foulant, sulfide. The sustainability of the catalyst was promising, as the catalyst was found to be stable under all conditions tested with respect to metal leaching. The presence of DO at concentrations typical of treatment conditions will increase H₂ demand for NO₃ ⁻ reduction, but has no negative impact on the selectivity of the catalyst. Under optimal conditions, i.e., a pH of 5.0 and a high NO₃ ⁻:H₂ influent loading, low NH₃ selectivity (5%) was achieved for extended periods (36 days), resulting in sustained levels of NH₃ that approached the European legal limit. The biggest challenge to the sustainability of the catalyst was the addition of sulfide, that initially increased NH₃ selectivity and ultimately resulted in complete deactivation of the catalyst. Further work is required to identify regeneration methods to restore sulfide-fouled catalyst activity and selectivity; however, the most effective use would be to remove sulfide prior to catalytic treatment.</description><subject>Aluminum oxide</subject><subject>Ammonia</subject><subject>Bimetals</subject><subject>Catalysis</subject><subject>Catalysts</subject><subject>Chemistry</subject><subject>Chemistry and Materials Science</subject><subject>Composition effects</subject><subject>Deactivation</subject><subject>Exact sciences and technology</subject><subject>Fouling</subject><subject>General and physical chemistry</subject><subject>Identification methods</subject><subject>Industrial Chemistry/Chemical Engineering</subject><subject>Leaching</subject><subject>Organometallic Chemistry</subject><subject>Palladium</subject><subject>Physical Chemistry</subject><subject>Reduction</subject><subject>Regeneration</subject><subject>Selectivity</subject><subject>Sustainability</subject><subject>Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry</subject><subject>Transitional aluminas</subject><issn>1011-372X</issn><issn>1572-879X</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2009</creationdate><recordtype>article</recordtype><sourceid>AFKRA</sourceid><sourceid>BENPR</sourceid><sourceid>CCPQU</sourceid><sourceid>DWQXO</sourceid><recordid>eNp9kM9qFTEUhwexYK0-gCsD4jI2J_Mnibt6qVootPS20F04N8nU1OnkmuQWLu6uj-R7-BB9EjNM0V1XOSTf78vhV1VvgH0AxsRhAtZ2nDKmqJKyps2zah9awakU6vp5mRkArQW_flG9TOmWFVCA2q9-Lt3gTPb3Pm8JjpYsNymjH3Hlh-kq9ATJuaUn4-Gf3_RoeNjtzh52v8gCMw7blIkfJwDNd2fpJ2fJhUOTQ_xILr85ctz3RT5JlmHYZB9Gsgh365D8NL-q9nocknv9eB5UV5-PLxdf6enZl5PF0Sk1NWOZdquyvFWNkyCsUR0XwirJjDAta1wvWSMMNwIsNithGuSutwCdkJ00NQpeH1TvZu86hh8bl7K-DZs4li81561UHRPQFgpmysSQUnS9Xkd_h3GrgempYz13rEt1eupYNyXz_tGMyeDQRxyNT_-CHDolm3bi-Myl8jTeuPh_g6fkb-dQj0HjTSziqyVnUDPoalCyrf8CWQCWjA</recordid><startdate>20090601</startdate><enddate>20090601</enddate><creator>Chaplin, Brian P</creator><creator>Shapley, John R</creator><creator>Werth, Charles J</creator><general>Boston : Springer US</general><general>Springer US</general><general>Springer</general><general>Springer Nature B.V</general><scope>FBQ</scope><scope>IQODW</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>8FE</scope><scope>8FG</scope><scope>ABJCF</scope><scope>AFKRA</scope><scope>BENPR</scope><scope>BGLVJ</scope><scope>CCPQU</scope><scope>D1I</scope><scope>DWQXO</scope><scope>HCIFZ</scope><scope>KB.</scope><scope>PDBOC</scope><scope>PQEST</scope><scope>PQQKQ</scope><scope>PQUKI</scope><scope>PRINS</scope></search><sort><creationdate>20090601</creationdate><title>Selectivity and Sustainability of a Pd-In/γ-Al₂O₃ Catalyst in a Packed-Bed Reactor: The Effect of Solution Composition</title><author>Chaplin, Brian P ; Shapley, John R ; Werth, Charles J</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c300t-6b101d94e817dc96277d980c7c504ef8047c2c71da4b7c4a2efd1167868c3a723</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2009</creationdate><topic>Aluminum oxide</topic><topic>Ammonia</topic><topic>Bimetals</topic><topic>Catalysis</topic><topic>Catalysts</topic><topic>Chemistry</topic><topic>Chemistry and Materials Science</topic><topic>Composition effects</topic><topic>Deactivation</topic><topic>Exact sciences and technology</topic><topic>Fouling</topic><topic>General and physical chemistry</topic><topic>Identification methods</topic><topic>Industrial Chemistry/Chemical Engineering</topic><topic>Leaching</topic><topic>Organometallic Chemistry</topic><topic>Palladium</topic><topic>Physical Chemistry</topic><topic>Reduction</topic><topic>Regeneration</topic><topic>Selectivity</topic><topic>Sustainability</topic><topic>Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry</topic><topic>Transitional aluminas</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Chaplin, Brian P</creatorcontrib><creatorcontrib>Shapley, John R</creatorcontrib><creatorcontrib>Werth, Charles J</creatorcontrib><collection>AGRIS</collection><collection>Pascal-Francis</collection><collection>CrossRef</collection><collection>ProQuest SciTech Collection</collection><collection>ProQuest Technology Collection</collection><collection>Materials Science & Engineering Collection</collection><collection>ProQuest Central UK/Ireland</collection><collection>ProQuest Central</collection><collection>Technology Collection</collection><collection>ProQuest One Community College</collection><collection>ProQuest Materials Science Collection</collection><collection>ProQuest Central Korea</collection><collection>SciTech Premium Collection</collection><collection>Materials Science Database</collection><collection>Materials Science Collection</collection><collection>ProQuest One Academic Eastern Edition (DO NOT USE)</collection><collection>ProQuest One Academic</collection><collection>ProQuest One Academic UKI Edition</collection><collection>ProQuest Central China</collection><jtitle>Catalysis letters</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Chaplin, Brian P</au><au>Shapley, John R</au><au>Werth, Charles J</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Selectivity and Sustainability of a Pd-In/γ-Al₂O₃ Catalyst in a Packed-Bed Reactor: The Effect of Solution Composition</atitle><jtitle>Catalysis letters</jtitle><stitle>Catal Lett</stitle><date>2009-06-01</date><risdate>2009</risdate><volume>130</volume><issue>1-2</issue><spage>56</spage><epage>62</epage><pages>56-62</pages><issn>1011-372X</issn><eissn>1572-879X</eissn><abstract>This study tested the selectivity and sustainability of an alumina-supported Pd-In bimetallic catalyst for nitrate reduction with H₂ in a continuous-flow packed-bed reactor in the presence of: (i) dissolved oxygen (DO), an alternative electron acceptor to nitrate, (ii) variable NO₃ ⁻:H₂ influent loadings, and (iii) the presence of a known foulant, sulfide. The sustainability of the catalyst was promising, as the catalyst was found to be stable under all conditions tested with respect to metal leaching. The presence of DO at concentrations typical of treatment conditions will increase H₂ demand for NO₃ ⁻ reduction, but has no negative impact on the selectivity of the catalyst. Under optimal conditions, i.e., a pH of 5.0 and a high NO₃ ⁻:H₂ influent loading, low NH₃ selectivity (5%) was achieved for extended periods (36 days), resulting in sustained levels of NH₃ that approached the European legal limit. The biggest challenge to the sustainability of the catalyst was the addition of sulfide, that initially increased NH₃ selectivity and ultimately resulted in complete deactivation of the catalyst. Further work is required to identify regeneration methods to restore sulfide-fouled catalyst activity and selectivity; however, the most effective use would be to remove sulfide prior to catalytic treatment.</abstract><cop>Boston</cop><pub>Boston : Springer US</pub><doi>10.1007/s10562-009-9883-4</doi><tpages>7</tpages></addata></record> |
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subjects | Aluminum oxide Ammonia Bimetals Catalysis Catalysts Chemistry Chemistry and Materials Science Composition effects Deactivation Exact sciences and technology Fouling General and physical chemistry Identification methods Industrial Chemistry/Chemical Engineering Leaching Organometallic Chemistry Palladium Physical Chemistry Reduction Regeneration Selectivity Sustainability Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry Transitional aluminas |
title | Selectivity and Sustainability of a Pd-In/γ-Al₂O₃ Catalyst in a Packed-Bed Reactor: The Effect of Solution Composition |
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