Novel catalytic and mechanistic studies on wastewater denitrification with hydrogen
The present work reports up-to-date information regarding the reaction mechanism of the catalytic hydrogenation of nitrates in water media. In the present mechanistic study, an attempt is made, for the first time, to elucidate the crucial role of several catalysts and reaction parameters in the mech...
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| Veröffentlicht in: | Water science and technology 2014-01, Vol.69 (3), p.680-686 |
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| creator | THEOLOGIDES, C. P OLYMPIOU, G. G SAVVA, P. G PANTELIDOU, N. A CONSTANTINOU, B. K CHATZIIONA, V. K VALANIDOU, L. Y PISKOPIANOU, C. T COSTA, C. N |
| description | The present work reports up-to-date information regarding the reaction mechanism of the catalytic hydrogenation of nitrates in water media. In the present mechanistic study, an attempt is made, for the first time, to elucidate the crucial role of several catalysts and reaction parameters in the mechanism of the NO(3)(-)/H(2) reaction. Steady-state isotopic transient kinetic analysis (SSITKA) experiments coupled with ex situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) were performed on supported Pd-Cu catalysts for the NO(3)(-)/H(2) and NO(3)(-)/H(2)/O(2) reactions. The latter experiments revealed that the formation and surface coverage of various adsorbed active intermediate N-species on the support or Pd/Cu metal surface is significantly favored in the presence of TiO(2) in the support mixture and in the presence of oxygen in the reaction's gaseous feed stream. The differences in the reactivity of these adsorbed N-species, found in the present work, adequately explain the large effect of the chemical composition of the support and the gas feed composition on catalyst behaviour (activity and selectivity). The present study leads to solid mechanistic evidence concerning the presence of a hydrogen spillover process from the metal to the support. Moreover, this study shows that Cu clusters are active sites for the reduction of nitrates to nitrites. |
| doi_str_mv | 10.2166/wst.2013.781 |
| format | Article |
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P ; OLYMPIOU, G. G ; SAVVA, P. G ; PANTELIDOU, N. A ; CONSTANTINOU, B. K ; CHATZIIONA, V. K ; VALANIDOU, L. Y ; PISKOPIANOU, C. T ; COSTA, C. N</creator><creatorcontrib>THEOLOGIDES, C. P ; OLYMPIOU, G. G ; SAVVA, P. G ; PANTELIDOU, N. A ; CONSTANTINOU, B. K ; CHATZIIONA, V. K ; VALANIDOU, L. Y ; PISKOPIANOU, C. T ; COSTA, C. N</creatorcontrib><description>The present work reports up-to-date information regarding the reaction mechanism of the catalytic hydrogenation of nitrates in water media. In the present mechanistic study, an attempt is made, for the first time, to elucidate the crucial role of several catalysts and reaction parameters in the mechanism of the NO(3)(-)/H(2) reaction. Steady-state isotopic transient kinetic analysis (SSITKA) experiments coupled with ex situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) were performed on supported Pd-Cu catalysts for the NO(3)(-)/H(2) and NO(3)(-)/H(2)/O(2) reactions. The latter experiments revealed that the formation and surface coverage of various adsorbed active intermediate N-species on the support or Pd/Cu metal surface is significantly favored in the presence of TiO(2) in the support mixture and in the presence of oxygen in the reaction's gaseous feed stream. The differences in the reactivity of these adsorbed N-species, found in the present work, adequately explain the large effect of the chemical composition of the support and the gas feed composition on catalyst behaviour (activity and selectivity). The present study leads to solid mechanistic evidence concerning the presence of a hydrogen spillover process from the metal to the support. Moreover, this study shows that Cu clusters are active sites for the reduction of nitrates to nitrites.</description><identifier>ISSN: 0273-1223</identifier><identifier>EISSN: 1996-9732</identifier><identifier>DOI: 10.2166/wst.2013.781</identifier><identifier>PMID: 24552744</identifier><identifier>CODEN: WSTED4</identifier><language>eng</language><publisher>London: International Water Association</publisher><subject>Analysis methods ; Analytical methods ; Applied sciences ; Catalysis ; Catalysts ; Composition effects ; Copper ; Copper - chemistry ; Denitrification ; Diffuse reflectance spectroscopy ; Exact sciences and technology ; Feed composition ; Feeds ; Fourier transforms ; General purification processes ; Hydrogen - chemistry ; Hydrogen storage ; Infrared analysis ; Metals ; Natural water pollution ; Nitrates ; Nitrites ; Nitrogen - chemistry ; Palladium ; Palladium - chemistry ; Pollution ; Reaction mechanisms ; Reflectance ; Selectivity ; Spectroscopy, Fourier Transform Infrared ; Titanium dioxide ; Waste Water - chemistry ; Wastewater ; Wastewaters ; Water treatment and pollution</subject><ispartof>Water science and technology, 2014-01, Vol.69 (3), p.680-686</ispartof><rights>2015 INIST-CNRS</rights><rights>Copyright IWA Publishing Feb 2014</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c316t-2679ad065aa9d54373c967ee3921c76df67b2e69bbab62fb8564fff5c98266af3</citedby></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,780,784,27924,27925</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=28323094$$DView record in Pascal Francis$$Hfree_for_read</backlink><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/24552744$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>THEOLOGIDES, C. P</creatorcontrib><creatorcontrib>OLYMPIOU, G. G</creatorcontrib><creatorcontrib>SAVVA, P. G</creatorcontrib><creatorcontrib>PANTELIDOU, N. A</creatorcontrib><creatorcontrib>CONSTANTINOU, B. K</creatorcontrib><creatorcontrib>CHATZIIONA, V. K</creatorcontrib><creatorcontrib>VALANIDOU, L. Y</creatorcontrib><creatorcontrib>PISKOPIANOU, C. T</creatorcontrib><creatorcontrib>COSTA, C. N</creatorcontrib><title>Novel catalytic and mechanistic studies on wastewater denitrification with hydrogen</title><title>Water science and technology</title><addtitle>Water Sci Technol</addtitle><description>The present work reports up-to-date information regarding the reaction mechanism of the catalytic hydrogenation of nitrates in water media. In the present mechanistic study, an attempt is made, for the first time, to elucidate the crucial role of several catalysts and reaction parameters in the mechanism of the NO(3)(-)/H(2) reaction. Steady-state isotopic transient kinetic analysis (SSITKA) experiments coupled with ex situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) were performed on supported Pd-Cu catalysts for the NO(3)(-)/H(2) and NO(3)(-)/H(2)/O(2) reactions. The latter experiments revealed that the formation and surface coverage of various adsorbed active intermediate N-species on the support or Pd/Cu metal surface is significantly favored in the presence of TiO(2) in the support mixture and in the presence of oxygen in the reaction's gaseous feed stream. The differences in the reactivity of these adsorbed N-species, found in the present work, adequately explain the large effect of the chemical composition of the support and the gas feed composition on catalyst behaviour (activity and selectivity). The present study leads to solid mechanistic evidence concerning the presence of a hydrogen spillover process from the metal to the support. Moreover, this study shows that Cu clusters are active sites for the reduction of nitrates to nitrites.</description><subject>Analysis methods</subject><subject>Analytical methods</subject><subject>Applied sciences</subject><subject>Catalysis</subject><subject>Catalysts</subject><subject>Composition effects</subject><subject>Copper</subject><subject>Copper - chemistry</subject><subject>Denitrification</subject><subject>Diffuse reflectance spectroscopy</subject><subject>Exact sciences and technology</subject><subject>Feed composition</subject><subject>Feeds</subject><subject>Fourier transforms</subject><subject>General purification processes</subject><subject>Hydrogen - chemistry</subject><subject>Hydrogen storage</subject><subject>Infrared analysis</subject><subject>Metals</subject><subject>Natural water pollution</subject><subject>Nitrates</subject><subject>Nitrites</subject><subject>Nitrogen - chemistry</subject><subject>Palladium</subject><subject>Palladium - chemistry</subject><subject>Pollution</subject><subject>Reaction mechanisms</subject><subject>Reflectance</subject><subject>Selectivity</subject><subject>Spectroscopy, Fourier Transform Infrared</subject><subject>Titanium dioxide</subject><subject>Waste Water - chemistry</subject><subject>Wastewater</subject><subject>Wastewaters</subject><subject>Water treatment and pollution</subject><issn>0273-1223</issn><issn>1996-9732</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2014</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><sourceid>ABUWG</sourceid><sourceid>AFKRA</sourceid><sourceid>BENPR</sourceid><sourceid>CCPQU</sourceid><sourceid>DWQXO</sourceid><recordid>eNpFkEtLAzEURoMotlZ3rmVA3Dk1r0mapRRfUHShrkMmD5syndEkY-m_N0Orri6Xe-73wQHgHMEpRozdbGKaYojIlM_QARgjIVgpOMGHYAwxJyXCmIzASYwrCCEnFB6DEaZVhTmlY_D63H3bptAqqWabvC5Ua4q11UvV-jjsMfXG21h0bbFRMdmNSjYUxrY-Be98fvTDyadlsdya0H3Y9hQcOdVEe7afE_B-f_c2fywXLw9P89tFqQliqcSMC2Ugq5QSpqKEEy0Yt5YIjDRnxjFeY8tEXauaYVfPKkadc5UWM8yYcmQCLne5n6H76m1MctX1oc2VEglKGKcc0kxd7ygduhiDdfIz-LUKW4mgHAzKbFAOBmU2mPGLfWhfr635g3-VZeBqD6ioVeOCarWP_9yMYAJz_Q_kSno3</recordid><startdate>20140101</startdate><enddate>20140101</enddate><creator>THEOLOGIDES, C. 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P</au><au>OLYMPIOU, G. G</au><au>SAVVA, P. G</au><au>PANTELIDOU, N. A</au><au>CONSTANTINOU, B. K</au><au>CHATZIIONA, V. K</au><au>VALANIDOU, L. Y</au><au>PISKOPIANOU, C. T</au><au>COSTA, C. N</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Novel catalytic and mechanistic studies on wastewater denitrification with hydrogen</atitle><jtitle>Water science and technology</jtitle><addtitle>Water Sci Technol</addtitle><date>2014-01-01</date><risdate>2014</risdate><volume>69</volume><issue>3</issue><spage>680</spage><epage>686</epage><pages>680-686</pages><issn>0273-1223</issn><eissn>1996-9732</eissn><coden>WSTED4</coden><abstract>The present work reports up-to-date information regarding the reaction mechanism of the catalytic hydrogenation of nitrates in water media. In the present mechanistic study, an attempt is made, for the first time, to elucidate the crucial role of several catalysts and reaction parameters in the mechanism of the NO(3)(-)/H(2) reaction. Steady-state isotopic transient kinetic analysis (SSITKA) experiments coupled with ex situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) were performed on supported Pd-Cu catalysts for the NO(3)(-)/H(2) and NO(3)(-)/H(2)/O(2) reactions. The latter experiments revealed that the formation and surface coverage of various adsorbed active intermediate N-species on the support or Pd/Cu metal surface is significantly favored in the presence of TiO(2) in the support mixture and in the presence of oxygen in the reaction's gaseous feed stream. The differences in the reactivity of these adsorbed N-species, found in the present work, adequately explain the large effect of the chemical composition of the support and the gas feed composition on catalyst behaviour (activity and selectivity). The present study leads to solid mechanistic evidence concerning the presence of a hydrogen spillover process from the metal to the support. Moreover, this study shows that Cu clusters are active sites for the reduction of nitrates to nitrites.</abstract><cop>London</cop><pub>International Water Association</pub><pmid>24552744</pmid><doi>10.2166/wst.2013.781</doi><tpages>7</tpages></addata></record> |
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| identifier | ISSN: 0273-1223 |
| ispartof | Water science and technology, 2014-01, Vol.69 (3), p.680-686 |
| issn | 0273-1223 1996-9732 |
| language | eng |
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| source | MEDLINE; EZB-FREE-00999 freely available EZB journals |
| subjects | Analysis methods Analytical methods Applied sciences Catalysis Catalysts Composition effects Copper Copper - chemistry Denitrification Diffuse reflectance spectroscopy Exact sciences and technology Feed composition Feeds Fourier transforms General purification processes Hydrogen - chemistry Hydrogen storage Infrared analysis Metals Natural water pollution Nitrates Nitrites Nitrogen - chemistry Palladium Palladium - chemistry Pollution Reaction mechanisms Reflectance Selectivity Spectroscopy, Fourier Transform Infrared Titanium dioxide Waste Water - chemistry Wastewater Wastewaters Water treatment and pollution |
| title | Novel catalytic and mechanistic studies on wastewater denitrification with hydrogen |
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