Experimental Study on the Effect of SO2 on PCDD/F Emissions: Determination of the Importance of Gas-Phase versus Solid-Phase Reactions in PCDD/F Formation
Cofiring coal in municipal solid waste incinerators (MSWIs) has previously been reported to reduce polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDDs/Fs) emissions due to increasing the flue gas SO2 concentration. The present study was focused on understanding the primary mechanism responsib...
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| Veröffentlicht in: | Environmental science & technology 2006-11, Vol.40 (22), p.7040-7047 |
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| creator | Ryan, Shawn P Li, Xiao-dong Gullett, Brian K Lee, C. W Clayton, Matt Touati, Abderrahmane |
| description | Cofiring coal in municipal solid waste incinerators (MSWIs) has previously been reported to reduce polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDDs/Fs) emissions due to increasing the flue gas SO2 concentration. The present study was focused on understanding the primary mechanism responsible for the suppressant effect of SO2 on total PCDD/F formation and toxic equivalent (TEQ) emissions. The addition of SO2, simulating the effect of coal addition on the flue gas composition, resulted in significant reductions in the TEQ emissions due to reactions involving SO2 in the postcombustion zone. However, emissions of total PCDDs/Fs, unlike the TEQ value, were dependent upon the Cl2 and SO2 injection temperatures due to increases in non-TEQ correlated isomers. The conversion of metal chlorides in the fly ash to sulfates, thus reducing the sites responsible for chlorination/oxidation reactions, was concluded to be the main suppressant mechanism; proposed reactions for copper and iron are presented. This mechanism was found to be independent of combustion conditions and could have prolonged effects on PCDD/F emissions from deposits formed with high flue gas S/Cl ratios. |
| doi_str_mv | 10.1021/es0615369 |
| format | Article |
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W ; Clayton, Matt ; Touati, Abderrahmane</creator><creatorcontrib>Ryan, Shawn P ; Li, Xiao-dong ; Gullett, Brian K ; Lee, C. W ; Clayton, Matt ; Touati, Abderrahmane</creatorcontrib><description>Cofiring coal in municipal solid waste incinerators (MSWIs) has previously been reported to reduce polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDDs/Fs) emissions due to increasing the flue gas SO2 concentration. The present study was focused on understanding the primary mechanism responsible for the suppressant effect of SO2 on total PCDD/F formation and toxic equivalent (TEQ) emissions. The addition of SO2, simulating the effect of coal addition on the flue gas composition, resulted in significant reductions in the TEQ emissions due to reactions involving SO2 in the postcombustion zone. However, emissions of total PCDDs/Fs, unlike the TEQ value, were dependent upon the Cl2 and SO2 injection temperatures due to increases in non-TEQ correlated isomers. The conversion of metal chlorides in the fly ash to sulfates, thus reducing the sites responsible for chlorination/oxidation reactions, was concluded to be the main suppressant mechanism; proposed reactions for copper and iron are presented. This mechanism was found to be independent of combustion conditions and could have prolonged effects on PCDD/F emissions from deposits formed with high flue gas S/Cl ratios.</description><identifier>ISSN: 0013-936X</identifier><identifier>EISSN: 1520-5851</identifier><identifier>DOI: 10.1021/es0615369</identifier><identifier>PMID: 17154014</identifier><identifier>CODEN: ESTHAG</identifier><language>eng</language><publisher>Washington, DC: American Chemical Society</publisher><subject>Air Pollution - analysis ; Applied sciences ; Atmospheric pollution ; Benzofurans - analysis ; Benzofurans - chemistry ; Coal ; Combustion and energy production ; Dibenzofurans, Polychlorinated ; Dioxins ; Emissions ; Exact sciences and technology ; Flue gas ; Gases ; Incineration ; Incinerators ; Municipal solid waste ; Pollution ; Pollution sources. Measurement results ; Polychlorinated Dibenzodioxins - analogs & derivatives ; Polychlorinated Dibenzodioxins - analysis ; Polychlorinated Dibenzodioxins - chemistry ; Refuse Disposal - methods ; Sulfur Dioxide - chemistry</subject><ispartof>Environmental science & technology, 2006-11, Vol.40 (22), p.7040-7047</ispartof><rights>Copyright © 2006 American Chemical Society</rights><rights>2007 INIST-CNRS</rights><rights>Copyright American Chemical Society Nov 15, 2006</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/es0615369$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/es0615369$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>315,782,786,27083,27931,27932,56745,56795</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=18290269$$DView record in Pascal Francis$$Hfree_for_read</backlink><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/17154014$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Ryan, Shawn P</creatorcontrib><creatorcontrib>Li, Xiao-dong</creatorcontrib><creatorcontrib>Gullett, Brian K</creatorcontrib><creatorcontrib>Lee, C. W</creatorcontrib><creatorcontrib>Clayton, Matt</creatorcontrib><creatorcontrib>Touati, Abderrahmane</creatorcontrib><title>Experimental Study on the Effect of SO2 on PCDD/F Emissions: Determination of the Importance of Gas-Phase versus Solid-Phase Reactions in PCDD/F Formation</title><title>Environmental science & technology</title><addtitle>Environ. Sci. Technol</addtitle><description>Cofiring coal in municipal solid waste incinerators (MSWIs) has previously been reported to reduce polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDDs/Fs) emissions due to increasing the flue gas SO2 concentration. The present study was focused on understanding the primary mechanism responsible for the suppressant effect of SO2 on total PCDD/F formation and toxic equivalent (TEQ) emissions. The addition of SO2, simulating the effect of coal addition on the flue gas composition, resulted in significant reductions in the TEQ emissions due to reactions involving SO2 in the postcombustion zone. However, emissions of total PCDDs/Fs, unlike the TEQ value, were dependent upon the Cl2 and SO2 injection temperatures due to increases in non-TEQ correlated isomers. The conversion of metal chlorides in the fly ash to sulfates, thus reducing the sites responsible for chlorination/oxidation reactions, was concluded to be the main suppressant mechanism; proposed reactions for copper and iron are presented. This mechanism was found to be independent of combustion conditions and could have prolonged effects on PCDD/F emissions from deposits formed with high flue gas S/Cl ratios.</description><subject>Air Pollution - analysis</subject><subject>Applied sciences</subject><subject>Atmospheric pollution</subject><subject>Benzofurans - analysis</subject><subject>Benzofurans - chemistry</subject><subject>Coal</subject><subject>Combustion and energy production</subject><subject>Dibenzofurans, Polychlorinated</subject><subject>Dioxins</subject><subject>Emissions</subject><subject>Exact sciences and technology</subject><subject>Flue gas</subject><subject>Gases</subject><subject>Incineration</subject><subject>Incinerators</subject><subject>Municipal solid waste</subject><subject>Pollution</subject><subject>Pollution sources. Measurement results</subject><subject>Polychlorinated Dibenzodioxins - analogs & derivatives</subject><subject>Polychlorinated Dibenzodioxins - analysis</subject><subject>Polychlorinated Dibenzodioxins - chemistry</subject><subject>Refuse Disposal - methods</subject><subject>Sulfur Dioxide - chemistry</subject><issn>0013-936X</issn><issn>1520-5851</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2006</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNpFkdtu1DAQhi0EokvhgheoLCQu044POfWu2lMriroiBXFnOc5ETbtJFttB7R23PERfrk9Shy67NzPS72_-sf4h5CODYwacnaCDhMUiyV-RCYs5RHEWs9dkAsBElIvk5wF559wtAHAB2VtywFIWS2ByQh7n9xu0TYud12ta-KF6oH1H_Q3SeV2j8bSvaXHFR3E1nc1OFnTeNs41fedOn_78pTP0aNum0z5IIzyOXrSb3nrdGRyVpXbR6kY7pL_RusHRol831Vb6htqMo442uw2L3rb__N6TN7VeO_yw7Yfk-2J-PT2PLq-WF9Ozy0hLAB9pUdYC68owJhG0zI0RWSIFGpmWUrLYlKbkaZllktVppUHwDLiOAask1Eockk8vvhvb_xrQeXXbD7YLK1VIjCUgMh6goy00lC1WahNi0_ZB_Q8zAJ-3gHZGr2sbAmjcnst4DjzJAxe9cI3zeL971_ZOJalIY3W9KtQX-CEKcb5UX_e-2rj9xxio8fhqd3zxDByYnWI</recordid><startdate>20061115</startdate><enddate>20061115</enddate><creator>Ryan, Shawn P</creator><creator>Li, Xiao-dong</creator><creator>Gullett, Brian K</creator><creator>Lee, C. W</creator><creator>Clayton, Matt</creator><creator>Touati, Abderrahmane</creator><general>American Chemical Society</general><scope>BSCLL</scope><scope>IQODW</scope><scope>CGR</scope><scope>CUY</scope><scope>CVF</scope><scope>ECM</scope><scope>EIF</scope><scope>NPM</scope><scope>7QO</scope><scope>7ST</scope><scope>7T7</scope><scope>7U7</scope><scope>8FD</scope><scope>C1K</scope><scope>FR3</scope><scope>P64</scope><scope>SOI</scope></search><sort><creationdate>20061115</creationdate><title>Experimental Study on the Effect of SO2 on PCDD/F Emissions: Determination of the Importance of Gas-Phase versus Solid-Phase Reactions in PCDD/F Formation</title><author>Ryan, Shawn P ; Li, Xiao-dong ; Gullett, Brian K ; Lee, C. W ; Clayton, Matt ; Touati, Abderrahmane</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a400t-a3bf3efdc114e0a49cc38643ec47b4415cbcb27b8841f7da032802a50ed6a50d3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2006</creationdate><topic>Air Pollution - analysis</topic><topic>Applied sciences</topic><topic>Atmospheric pollution</topic><topic>Benzofurans - analysis</topic><topic>Benzofurans - chemistry</topic><topic>Coal</topic><topic>Combustion and energy production</topic><topic>Dibenzofurans, Polychlorinated</topic><topic>Dioxins</topic><topic>Emissions</topic><topic>Exact sciences and technology</topic><topic>Flue gas</topic><topic>Gases</topic><topic>Incineration</topic><topic>Incinerators</topic><topic>Municipal solid waste</topic><topic>Pollution</topic><topic>Pollution sources. Measurement results</topic><topic>Polychlorinated Dibenzodioxins - analogs & derivatives</topic><topic>Polychlorinated Dibenzodioxins - analysis</topic><topic>Polychlorinated Dibenzodioxins - chemistry</topic><topic>Refuse Disposal - methods</topic><topic>Sulfur Dioxide - chemistry</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Ryan, Shawn P</creatorcontrib><creatorcontrib>Li, Xiao-dong</creatorcontrib><creatorcontrib>Gullett, Brian K</creatorcontrib><creatorcontrib>Lee, C. W</creatorcontrib><creatorcontrib>Clayton, Matt</creatorcontrib><creatorcontrib>Touati, Abderrahmane</creatorcontrib><collection>Istex</collection><collection>Pascal-Francis</collection><collection>Medline</collection><collection>MEDLINE</collection><collection>MEDLINE (Ovid)</collection><collection>MEDLINE</collection><collection>MEDLINE</collection><collection>PubMed</collection><collection>Biotechnology Research Abstracts</collection><collection>Environment Abstracts</collection><collection>Industrial and Applied Microbiology Abstracts (Microbiology A)</collection><collection>Toxicology Abstracts</collection><collection>Technology Research Database</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Engineering Research Database</collection><collection>Biotechnology and BioEngineering Abstracts</collection><collection>Environment Abstracts</collection><jtitle>Environmental science & technology</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Ryan, Shawn P</au><au>Li, Xiao-dong</au><au>Gullett, Brian K</au><au>Lee, C. W</au><au>Clayton, Matt</au><au>Touati, Abderrahmane</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Experimental Study on the Effect of SO2 on PCDD/F Emissions: Determination of the Importance of Gas-Phase versus Solid-Phase Reactions in PCDD/F Formation</atitle><jtitle>Environmental science & technology</jtitle><addtitle>Environ. Sci. Technol</addtitle><date>2006-11-15</date><risdate>2006</risdate><volume>40</volume><issue>22</issue><spage>7040</spage><epage>7047</epage><pages>7040-7047</pages><issn>0013-936X</issn><eissn>1520-5851</eissn><coden>ESTHAG</coden><abstract>Cofiring coal in municipal solid waste incinerators (MSWIs) has previously been reported to reduce polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDDs/Fs) emissions due to increasing the flue gas SO2 concentration. The present study was focused on understanding the primary mechanism responsible for the suppressant effect of SO2 on total PCDD/F formation and toxic equivalent (TEQ) emissions. The addition of SO2, simulating the effect of coal addition on the flue gas composition, resulted in significant reductions in the TEQ emissions due to reactions involving SO2 in the postcombustion zone. However, emissions of total PCDDs/Fs, unlike the TEQ value, were dependent upon the Cl2 and SO2 injection temperatures due to increases in non-TEQ correlated isomers. The conversion of metal chlorides in the fly ash to sulfates, thus reducing the sites responsible for chlorination/oxidation reactions, was concluded to be the main suppressant mechanism; proposed reactions for copper and iron are presented. This mechanism was found to be independent of combustion conditions and could have prolonged effects on PCDD/F emissions from deposits formed with high flue gas S/Cl ratios.</abstract><cop>Washington, DC</cop><pub>American Chemical Society</pub><pmid>17154014</pmid><doi>10.1021/es0615369</doi><tpages>8</tpages></addata></record> |
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| ispartof | Environmental science & technology, 2006-11, Vol.40 (22), p.7040-7047 |
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| subjects | Air Pollution - analysis Applied sciences Atmospheric pollution Benzofurans - analysis Benzofurans - chemistry Coal Combustion and energy production Dibenzofurans, Polychlorinated Dioxins Emissions Exact sciences and technology Flue gas Gases Incineration Incinerators Municipal solid waste Pollution Pollution sources. Measurement results Polychlorinated Dibenzodioxins - analogs & derivatives Polychlorinated Dibenzodioxins - analysis Polychlorinated Dibenzodioxins - chemistry Refuse Disposal - methods Sulfur Dioxide - chemistry |
| title | Experimental Study on the Effect of SO2 on PCDD/F Emissions: Determination of the Importance of Gas-Phase versus Solid-Phase Reactions in PCDD/F Formation |
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