Atmospheric Chemistry of Perfluoroaldehydes (C x F2 x +1CHO) and Fluorotelomer Aldehydes (C x F2 x +1CH2CHO): Quantification of the Important Role of Photolysis
The UV absorption spectra of CF3CHO, C2F5CHO, C3F7CHO, C4F9CHO, CF3CH2CHO, and C6F13CH2CHO were recorded over the range 225−400 nm at 249−297 K. C x F2 x +1CHO and C x F2 x +1CH2CHO have broad absorption features centered at 300−310 and 290−300 nm, respectively. The strength of the absorption increa...
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| Veröffentlicht in: | The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory Molecules, spectroscopy, kinetics, environment, & general theory, 2006-11, Vol.110 (43), p.11944-11953 |
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| container_title | The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory |
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| creator | Chiappero, Malisa S Malanca, Fabio E Argüello, Gustavo A Wooldridge, Steven T Hurley, Michael D Ball, James C Wallington, Timothy J Waterland, Robert L Buck, Robert C |
| description | The UV absorption spectra of CF3CHO, C2F5CHO, C3F7CHO, C4F9CHO, CF3CH2CHO, and C6F13CH2CHO were recorded over the range 225−400 nm at 249−297 K. C x F2 x +1CHO and C x F2 x +1CH2CHO have broad absorption features centered at 300−310 and 290−300 nm, respectively. The strength of the absorption increases with the size of the C x F2 x +1 group. There was no discernible ( |
| doi_str_mv | 10.1021/jp064262k |
| format | Article |
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C x F2 x +1CHO and C x F2 x +1CH2CHO have broad absorption features centered at 300−310 and 290−300 nm, respectively. The strength of the absorption increases with the size of the C x F2 x +1 group. There was no discernible (<5%) effect of temperature on the UV spectra. Quantum yields for photolysis at 254 and 308 nm were measured. Quantum yields at 254 nm were 0.79 ± 0.09 (CF3CHO), 0.81 ± 0.09 (C2F5CHO), 0.63 ± 0.09 (C3F7CHO), 0.60 ± 0.09 (C4F9CHO), 0.74 ± 0.08 (CF3CH2CHO), and 0.55 ± 0.09 (C6F13CH2CHO). Quantum yields at 308 nm were 0.17 ± 0.03 (CF3CHO), 0.08 ± 0.02 (C4F9CHO), and 0.04 ± 0.01 (CF3CH2CHO). The quantum yields decrease with increasing size of the C x F2 x +1 group and with increasing wavelength of the photolysis light. The photolysis quantum yield at 308 nm for CF3CHO measured here is a factor of at least 8 greater than that reported previously. Photolysis is probably the dominant atmospheric fate of C x F2 x +1CHO (x = 1−4) and is an important fate of C x F2 x +1CH2CHO (x = 1 and 6). These results have important ramifications concerning the yield of perfluorocarboxylic acids in the atmospheric oxidation of fluorotelomer alcohols.</description><identifier>ISSN: 1089-5639</identifier><identifier>EISSN: 1520-5215</identifier><identifier>DOI: 10.1021/jp064262k</identifier><identifier>PMID: 17064182</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><ispartof>The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory, 2006-11, Vol.110 (43), p.11944-11953</ispartof><rights>Copyright © 2006 American Chemical Society</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a351t-10d3ab38e22e8988582ff48b20a2ce6da35fdc8508d859ba9fad7b85514e43b63</citedby><cites>FETCH-LOGICAL-a351t-10d3ab38e22e8988582ff48b20a2ce6da35fdc8508d859ba9fad7b85514e43b63</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/jp064262k$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/jp064262k$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,780,784,2763,27075,27923,27924,56737,56787</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/17064182$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Chiappero, Malisa S</creatorcontrib><creatorcontrib>Malanca, Fabio E</creatorcontrib><creatorcontrib>Argüello, Gustavo A</creatorcontrib><creatorcontrib>Wooldridge, Steven T</creatorcontrib><creatorcontrib>Hurley, Michael D</creatorcontrib><creatorcontrib>Ball, James C</creatorcontrib><creatorcontrib>Wallington, Timothy J</creatorcontrib><creatorcontrib>Waterland, Robert L</creatorcontrib><creatorcontrib>Buck, Robert C</creatorcontrib><title>Atmospheric Chemistry of Perfluoroaldehydes (C x F2 x +1CHO) and Fluorotelomer Aldehydes (C x F2 x +1CH2CHO): Quantification of the Important Role of Photolysis</title><title>The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory</title><addtitle>J. Phys. Chem. A</addtitle><description>The UV absorption spectra of CF3CHO, C2F5CHO, C3F7CHO, C4F9CHO, CF3CH2CHO, and C6F13CH2CHO were recorded over the range 225−400 nm at 249−297 K. C x F2 x +1CHO and C x F2 x +1CH2CHO have broad absorption features centered at 300−310 and 290−300 nm, respectively. The strength of the absorption increases with the size of the C x F2 x +1 group. There was no discernible (<5%) effect of temperature on the UV spectra. Quantum yields for photolysis at 254 and 308 nm were measured. Quantum yields at 254 nm were 0.79 ± 0.09 (CF3CHO), 0.81 ± 0.09 (C2F5CHO), 0.63 ± 0.09 (C3F7CHO), 0.60 ± 0.09 (C4F9CHO), 0.74 ± 0.08 (CF3CH2CHO), and 0.55 ± 0.09 (C6F13CH2CHO). Quantum yields at 308 nm were 0.17 ± 0.03 (CF3CHO), 0.08 ± 0.02 (C4F9CHO), and 0.04 ± 0.01 (CF3CH2CHO). The quantum yields decrease with increasing size of the C x F2 x +1 group and with increasing wavelength of the photolysis light. The photolysis quantum yield at 308 nm for CF3CHO measured here is a factor of at least 8 greater than that reported previously. Photolysis is probably the dominant atmospheric fate of C x F2 x +1CHO (x = 1−4) and is an important fate of C x F2 x +1CH2CHO (x = 1 and 6). These results have important ramifications concerning the yield of perfluorocarboxylic acids in the atmospheric oxidation of fluorotelomer alcohols.</description><issn>1089-5639</issn><issn>1520-5215</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2006</creationdate><recordtype>article</recordtype><recordid>eNp10c1u1DAQB3ALgWgpHHgB5AuICgX8ESdOb7sR21YqtJRytpxkrGSbxMF2pO6NK8_Bm_EkeLurcoGLbWl-npH-g9BLSt5TwuiH9USylGXs9hE6pIKRRDAqHsc3kUUiMl4coGferwkhlLP0KTqgefxAJTtEvxZhsH5qwXU1LlsYOh_cBluDr8CZfrbO6r6BdtOAx29LfIdXLB7vaHl2eYz12ODVPQrQ2wEcXvwHs60_-f3jJ_4y6zF0pqt16Oy4nRRawOfDZF2IFXxte7if39pg-43v_HP0xOjew4v9fYS-rT7elGfJxeXpebm4SDQXNCSUNFxXXAJjIAsphWTGpLJiRLMasiYq09RSENlIUVS6MLrJKykETSHlVcaP0Jtd38nZ7zP4oGIaNfS9HsHOXmWyKNKC5hEe72DtrPcOjJpcN2i3UZSo7UbUw0aifbVvOlcDNH_lfgURJDsQk4e7h7p2tyrLeS7UzdVXxT99Xp7y5bVaRv9653Xt1drOboyZ_GPwH-FvoUo</recordid><startdate>20061102</startdate><enddate>20061102</enddate><creator>Chiappero, Malisa S</creator><creator>Malanca, Fabio E</creator><creator>Argüello, Gustavo A</creator><creator>Wooldridge, Steven T</creator><creator>Hurley, Michael D</creator><creator>Ball, James C</creator><creator>Wallington, Timothy J</creator><creator>Waterland, Robert L</creator><creator>Buck, Robert C</creator><general>American Chemical Society</general><scope>BSCLL</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope></search><sort><creationdate>20061102</creationdate><title>Atmospheric Chemistry of Perfluoroaldehydes (C x F2 x +1CHO) and Fluorotelomer Aldehydes (C x F2 x +1CH2CHO): Quantification of the Important Role of Photolysis</title><author>Chiappero, Malisa S ; Malanca, Fabio E ; Argüello, Gustavo A ; Wooldridge, Steven T ; Hurley, Michael D ; Ball, James C ; Wallington, Timothy J ; Waterland, Robert L ; Buck, Robert C</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a351t-10d3ab38e22e8988582ff48b20a2ce6da35fdc8508d859ba9fad7b85514e43b63</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2006</creationdate><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Chiappero, Malisa S</creatorcontrib><creatorcontrib>Malanca, Fabio E</creatorcontrib><creatorcontrib>Argüello, Gustavo A</creatorcontrib><creatorcontrib>Wooldridge, Steven T</creatorcontrib><creatorcontrib>Hurley, Michael D</creatorcontrib><creatorcontrib>Ball, James C</creatorcontrib><creatorcontrib>Wallington, Timothy J</creatorcontrib><creatorcontrib>Waterland, Robert L</creatorcontrib><creatorcontrib>Buck, Robert C</creatorcontrib><collection>Istex</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><jtitle>The journal of physical chemistry. 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A</addtitle><date>2006-11-02</date><risdate>2006</risdate><volume>110</volume><issue>43</issue><spage>11944</spage><epage>11953</epage><pages>11944-11953</pages><issn>1089-5639</issn><eissn>1520-5215</eissn><abstract>The UV absorption spectra of CF3CHO, C2F5CHO, C3F7CHO, C4F9CHO, CF3CH2CHO, and C6F13CH2CHO were recorded over the range 225−400 nm at 249−297 K. C x F2 x +1CHO and C x F2 x +1CH2CHO have broad absorption features centered at 300−310 and 290−300 nm, respectively. The strength of the absorption increases with the size of the C x F2 x +1 group. There was no discernible (<5%) effect of temperature on the UV spectra. Quantum yields for photolysis at 254 and 308 nm were measured. Quantum yields at 254 nm were 0.79 ± 0.09 (CF3CHO), 0.81 ± 0.09 (C2F5CHO), 0.63 ± 0.09 (C3F7CHO), 0.60 ± 0.09 (C4F9CHO), 0.74 ± 0.08 (CF3CH2CHO), and 0.55 ± 0.09 (C6F13CH2CHO). Quantum yields at 308 nm were 0.17 ± 0.03 (CF3CHO), 0.08 ± 0.02 (C4F9CHO), and 0.04 ± 0.01 (CF3CH2CHO). The quantum yields decrease with increasing size of the C x F2 x +1 group and with increasing wavelength of the photolysis light. The photolysis quantum yield at 308 nm for CF3CHO measured here is a factor of at least 8 greater than that reported previously. Photolysis is probably the dominant atmospheric fate of C x F2 x +1CHO (x = 1−4) and is an important fate of C x F2 x +1CH2CHO (x = 1 and 6). These results have important ramifications concerning the yield of perfluorocarboxylic acids in the atmospheric oxidation of fluorotelomer alcohols.</abstract><cop>United States</cop><pub>American Chemical Society</pub><pmid>17064182</pmid><doi>10.1021/jp064262k</doi><tpages>10</tpages></addata></record> |
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| title | Atmospheric Chemistry of Perfluoroaldehydes (C x F2 x +1CHO) and Fluorotelomer Aldehydes (C x F2 x +1CH2CHO): Quantification of the Important Role of Photolysis |
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