Continued emissions of carbon tetrachloride from the United States nearly two decades after its phaseout for dispersive uses
National-scale emissions of carbon tetrachloride (CCl₄) are derived based on inverse modeling of atmospheric observations at multiple sites across the United States from the National Oceanic and Atmospheric Administration’s flask air sampling network. We estimate an annual average US emission of 4.0...
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creator | Hu, Lei Montzka, Stephen A. Miller, Ben R. Andrews, Arlyn E. Miller, John B. Lehman, Scott J. Sweeney, Colm Miller, Scot M. Thoning, Kirk Siso, Carolina Atlas, Elliot L. Blake, Donald R. de Gouw, Joost Gilman, Jessica B. Dutton, Geoff Elkins, James W. Hall, Bradley Chen, Huilin Fischer, Marc L. Mountain, Marikate E. Nehrkorn, Thomas Biraud, Sebastien C. Moore, Fred L. Tans, Pieter |
description | National-scale emissions of carbon tetrachloride (CCl₄) are derived based on inverse modeling of atmospheric observations at multiple sites across the United States from the National Oceanic and Atmospheric Administration’s flask air sampling network. We estimate an annual average US emission of 4.0 (2.0–6.5) Gg CCl₄ y−1 during 2008–2012, which is almost two orders of magnitude larger than reported to the US Environmental Protection Agency (EPA) Toxics Release Inventory (TRI) (mean of 0.06 Gg y−1) but only 8% (3–22%) of global CCl₄ emissions during these years. Emissive regions identified by the observations and consistently shown in all inversion results include the Gulf Coast states, the San Francisco Bay Area in California, and the Denver area in Colorado. Both the observation-derived emissions and the US EPA TRI identified Texas and Louisiana as the largest contributors, accounting for one- to two-thirds of the US national total CCl₄ emission during 2008–2012. These results are qualitatively consistent with multiple aircraft and ship surveys conducted in earlier years, which suggested significant enhancements in atmospheric mole fractions measured near Houston and surrounding areas. Furthermore, the emission distribution derived for CCl₄ throughout the United States is more consistent with the distribution of industrial activities included in the TRI than with the distribution of other potential CCl₄ sources such as uncapped landfills or activities related to population density (e.g., use of chlorine-containing bleach). |
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We estimate an annual average US emission of 4.0 (2.0–6.5) Gg CCl₄ y−1 during 2008–2012, which is almost two orders of magnitude larger than reported to the US Environmental Protection Agency (EPA) Toxics Release Inventory (TRI) (mean of 0.06 Gg y−1) but only 8% (3–22%) of global CCl₄ emissions during these years. Emissive regions identified by the observations and consistently shown in all inversion results include the Gulf Coast states, the San Francisco Bay Area in California, and the Denver area in Colorado. Both the observation-derived emissions and the US EPA TRI identified Texas and Louisiana as the largest contributors, accounting for one- to two-thirds of the US national total CCl₄ emission during 2008–2012. These results are qualitatively consistent with multiple aircraft and ship surveys conducted in earlier years, which suggested significant enhancements in atmospheric mole fractions measured near Houston and surrounding areas. Furthermore, the emission distribution derived for CCl₄ throughout the United States is more consistent with the distribution of industrial activities included in the TRI than with the distribution of other potential CCl₄ sources such as uncapped landfills or activities related to population density (e.g., use of chlorine-containing bleach).</description><identifier>ISSN: 0027-8424</identifier><identifier>EISSN: 1091-6490</identifier><identifier>DOI: 10.1073/pnas.1522284113</identifier><identifier>PMID: 26929368</identifier><language>eng</language><publisher>United States: National Academy of Sciences</publisher><subject>Air sampling ; Carbon ; Chlorine ; Emissions ; Environmental protection ; ENVIRONMENTAL SCIENCES ; GEOSCIENCES ; Industrial areas ; Landfills ; Physical Sciences ; Population density ; Waste disposal sites</subject><ispartof>Proceedings of the National Academy of Sciences - PNAS, 2016-03, Vol.113 (11), p.2880-2885</ispartof><rights>Volumes 1–89 and 106–113, copyright as a collective work only; author(s) retains copyright to individual articles</rights><rights>Copyright National Academy of Sciences Mar 15, 2016</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c527t-5c70594d4b085916903f2b07b8f74f6907f4aeeb7a7db4ccd402e3118a17e4c53</citedby><cites>FETCH-LOGICAL-c527t-5c70594d4b085916903f2b07b8f74f6907f4aeeb7a7db4ccd402e3118a17e4c53</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Uhttp://www.pnas.org/content/113/11.cover.gif</thumbnail><linktopdf>$$Uhttps://www.jstor.org/stable/pdf/26468663$$EPDF$$P50$$Gjstor$$H</linktopdf><linktohtml>$$Uhttps://www.jstor.org/stable/26468663$$EHTML$$P50$$Gjstor$$H</linktohtml><link.rule.ids>230,314,723,776,780,799,881,27901,27902,53766,53768,57992,58225</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/26929368$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink><backlink>$$Uhttps://www.osti.gov/servlets/purl/1471010$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Hu, Lei</creatorcontrib><creatorcontrib>Montzka, Stephen A.</creatorcontrib><creatorcontrib>Miller, Ben R.</creatorcontrib><creatorcontrib>Andrews, Arlyn E.</creatorcontrib><creatorcontrib>Miller, John B.</creatorcontrib><creatorcontrib>Lehman, Scott J.</creatorcontrib><creatorcontrib>Sweeney, Colm</creatorcontrib><creatorcontrib>Miller, Scot M.</creatorcontrib><creatorcontrib>Thoning, Kirk</creatorcontrib><creatorcontrib>Siso, Carolina</creatorcontrib><creatorcontrib>Atlas, Elliot L.</creatorcontrib><creatorcontrib>Blake, Donald R.</creatorcontrib><creatorcontrib>de Gouw, Joost</creatorcontrib><creatorcontrib>Gilman, Jessica B.</creatorcontrib><creatorcontrib>Dutton, Geoff</creatorcontrib><creatorcontrib>Elkins, James W.</creatorcontrib><creatorcontrib>Hall, Bradley</creatorcontrib><creatorcontrib>Chen, Huilin</creatorcontrib><creatorcontrib>Fischer, Marc L.</creatorcontrib><creatorcontrib>Mountain, Marikate E.</creatorcontrib><creatorcontrib>Nehrkorn, Thomas</creatorcontrib><creatorcontrib>Biraud, Sebastien C.</creatorcontrib><creatorcontrib>Moore, Fred L.</creatorcontrib><creatorcontrib>Tans, Pieter</creatorcontrib><creatorcontrib>Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)</creatorcontrib><title>Continued emissions of carbon tetrachloride from the United States nearly two decades after its phaseout for dispersive uses</title><title>Proceedings of the National Academy of Sciences - PNAS</title><addtitle>Proc Natl Acad Sci U S A</addtitle><description>National-scale emissions of carbon tetrachloride (CCl₄) are derived based on inverse modeling of atmospheric observations at multiple sites across the United States from the National Oceanic and Atmospheric Administration’s flask air sampling network. We estimate an annual average US emission of 4.0 (2.0–6.5) Gg CCl₄ y−1 during 2008–2012, which is almost two orders of magnitude larger than reported to the US Environmental Protection Agency (EPA) Toxics Release Inventory (TRI) (mean of 0.06 Gg y−1) but only 8% (3–22%) of global CCl₄ emissions during these years. Emissive regions identified by the observations and consistently shown in all inversion results include the Gulf Coast states, the San Francisco Bay Area in California, and the Denver area in Colorado. Both the observation-derived emissions and the US EPA TRI identified Texas and Louisiana as the largest contributors, accounting for one- to two-thirds of the US national total CCl₄ emission during 2008–2012. These results are qualitatively consistent with multiple aircraft and ship surveys conducted in earlier years, which suggested significant enhancements in atmospheric mole fractions measured near Houston and surrounding areas. Furthermore, the emission distribution derived for CCl₄ throughout the United States is more consistent with the distribution of industrial activities included in the TRI than with the distribution of other potential CCl₄ sources such as uncapped landfills or activities related to population density (e.g., use of chlorine-containing bleach).</description><subject>Air sampling</subject><subject>Carbon</subject><subject>Chlorine</subject><subject>Emissions</subject><subject>Environmental protection</subject><subject>ENVIRONMENTAL SCIENCES</subject><subject>GEOSCIENCES</subject><subject>Industrial areas</subject><subject>Landfills</subject><subject>Physical Sciences</subject><subject>Population density</subject><subject>Waste disposal 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James W.</au><au>Hall, Bradley</au><au>Chen, Huilin</au><au>Fischer, Marc L.</au><au>Mountain, Marikate E.</au><au>Nehrkorn, Thomas</au><au>Biraud, Sebastien C.</au><au>Moore, Fred L.</au><au>Tans, Pieter</au><aucorp>Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Continued emissions of carbon tetrachloride from the United States nearly two decades after its phaseout for dispersive uses</atitle><jtitle>Proceedings of the National Academy of Sciences - PNAS</jtitle><addtitle>Proc Natl Acad Sci U S A</addtitle><date>2016-03-15</date><risdate>2016</risdate><volume>113</volume><issue>11</issue><spage>2880</spage><epage>2885</epage><pages>2880-2885</pages><issn>0027-8424</issn><eissn>1091-6490</eissn><abstract>National-scale emissions of carbon tetrachloride (CCl₄) are derived based on inverse modeling of atmospheric observations at multiple sites across the United States from the National Oceanic and Atmospheric Administration’s flask air sampling network. We estimate an annual average US emission of 4.0 (2.0–6.5) Gg CCl₄ y−1 during 2008–2012, which is almost two orders of magnitude larger than reported to the US Environmental Protection Agency (EPA) Toxics Release Inventory (TRI) (mean of 0.06 Gg y−1) but only 8% (3–22%) of global CCl₄ emissions during these years. Emissive regions identified by the observations and consistently shown in all inversion results include the Gulf Coast states, the San Francisco Bay Area in California, and the Denver area in Colorado. Both the observation-derived emissions and the US EPA TRI identified Texas and Louisiana as the largest contributors, accounting for one- to two-thirds of the US national total CCl₄ emission during 2008–2012. These results are qualitatively consistent with multiple aircraft and ship surveys conducted in earlier years, which suggested significant enhancements in atmospheric mole fractions measured near Houston and surrounding areas. Furthermore, the emission distribution derived for CCl₄ throughout the United States is more consistent with the distribution of industrial activities included in the TRI than with the distribution of other potential CCl₄ sources such as uncapped landfills or activities related to population density (e.g., use of chlorine-containing bleach).</abstract><cop>United States</cop><pub>National Academy of Sciences</pub><pmid>26929368</pmid><doi>10.1073/pnas.1522284113</doi><tpages>6</tpages><oa>free_for_read</oa></addata></record> |
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subjects | Air sampling Carbon Chlorine Emissions Environmental protection ENVIRONMENTAL SCIENCES GEOSCIENCES Industrial areas Landfills Physical Sciences Population density Waste disposal sites |
title | Continued emissions of carbon tetrachloride from the United States nearly two decades after its phaseout for dispersive uses |
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