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首页> 外文期刊>Environmental Science & Technology >Atmospheric Oxidation of Vinyl and Allyl Acetate: Product Distribution and Mechanisms of the OH-Initiated Degradation in the Presence and Absence of NO_x
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Atmospheric Oxidation of Vinyl and Allyl Acetate: Product Distribution and Mechanisms of the OH-Initiated Degradation in the Presence and Absence of NO_x

机译：乙酸乙烯酯和乙酸烯丙酯的大气氧化：存在和不存在NO_x时OH降解的产物分布和机理

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摘要

The products formed from the reactions of OH radicals with vinyl acetate and allyl acetate have been studied in a 1080 L quartz-glass chamber in the presence and absence of NO, using in situ FTIR spectroscopy to monitor the reactant decay and product formation. The yields of the primary products formed in the reaction of OH with vinyl acetate were: formic acetic anhydride (84 ± 11)%; acetic acid (18 ± 3)% and formaldehyde (99 ± 15)% in the presence of NO, and formic acetic anhydride (28 ± 5)%; acetic acid (87 ± 12)% and formaldehyde (52 ± 8)% in the absence of NO,. For the reaction of OH with allyl acetate the yields of the identified products were: acetoxyacetaldehyde (96 ± 15)% and formaldehyde (90 ± 12)% in the presence of NO_x and acetoxyacetaldehyde (26 ± 4)% and formaldehyde (12 ± 3)% in the absence of NO,. The present results indicate that in the absence of NO_x the main fate of the 1,2-hydroxyalkoxy radicals formed after addition of OH to the double bond in the compounds is, in the case of vinyl acetate, an α-ester rearrangement to produce acetic acid and CH_2(OH)CO~· radicals and in the case of allyl acetate reaction of the radical with O_2 to form acetic acid 3-hydroxy-2-oxo-propyl ester (CH_3C(O)OCH_2C(O)-CH_2OH). In contrast, in the presence of NO, the main reaction pathway for the 1,2-hydroxyalkoxy radicals is decomposition. The results are compared with the available literature data and implications for the atmospheric chemistry of vinyl and allyl acetate are assessed.
机译：已经在存在和不存在NO的情况下，在1080 L石英玻璃室中研究了OH自由基与乙酸乙烯酯和乙酸烯丙酯反应形成的产物，并使用原位FTIR光谱法监测了反应物的衰变和产物的形成。在OH与乙酸乙烯酯的反应中形成的初级产物的产率为：甲酸乙酸酐（84±11）％；和一氧化氮存在下的乙酸（18±3）％和甲醛（99±15）％，以及甲酸乙酸酐（28±5）％;在没有NO的情况下，乙酸（87±12）％和甲醛（52±8）％。对于OH与乙酸烯丙酯的反应，鉴定出的产物的产率为：在NO_x和乙酰氧基乙醛（26±4）％和甲醛（12±3）存在下，乙酰氧基乙醛（96±15）％和甲醛（90±12）％ ）％在没有NO的情况下。本结果表明，在不存在NO_x的情况下，在化合物中将OH加成双键后形成的1，2-羟基烷氧基的主要结局是乙酸乙烯酯，其α-酯重排以产生乙酸。酸和CH_2（OH）CO〜·基团，并且在乙酸烯丙酯与O_2进行烯丙基乙酸酯反应的情况下，形成乙酸3-羟基-2-氧代丙酯（CH_3C（O）OCH_2C（O）-CH_2OH）。相反，在NO存在下，1,2-羟基烷氧基自由基的主要反应途径是分解。将结果与可用的文献数据进行比较，并对乙烯和乙酸烯丙酯的大气化学性质进行了评估。

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  • 来源
    《Environmental Science & Technology》 |2012年第16期|p.8817-8825|共9页
  • 作者

    Maria B. Blanco; Iustinian Bejan; Ian Barnes; Peter Wiesen; Mariano A. Teruel;

  • 作者单位

    Physikalische Chemie/FBC, Bergische Universitaet Wuppertal, Wuppertal, Germany,Instituto de Investigaciones en Fisicoquimica de Cordoba (I.N.F.L.Q.C), Departmento de Fisicoquimica, Facultad de Ciencias Quimicas, Universidad Nacional de Cordoba, Ciudad Universitaria, 5000 Cordoba, Argentina;

    Physikalische Chemie/FBC, Bergische Universitaet Wuppertal, Wuppertal, Germany,Al. I. Cuza' Faculty of Inorganic and Analytical Chemistry, University of Iasi, Iasi, Romania;

    Physikalische Chemie/FBC, Bergische Universitaet Wuppertal, Wuppertal, Germany;

    Physikalische Chemie/FBC, Bergische Universitaet Wuppertal, Wuppertal, Germany;

    Instituto de Investigaciones en Fisicoquimica de Cordoba (I.N.F.L.Q.C), Departmento de Fisicoquimica, Facultad de Ciencias Quimicas, Universidad Nacional de Cordoba, Ciudad Universitaria, 5000 Cordoba, Argentina;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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