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首页> 外文期刊>Environmental Science & Technology >Methyl-Perfluoroheptene-Ethers (CH_3OC_7F_(13)): Measured OH Radical Reaction Rate Coefficients for Several Isomers and Enantiomers and Their Atmospheric Lifetimes and Global Warming Potentials
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Methyl-Perfluoroheptene-Ethers (CH_3OC_7F_(13)): Measured OH Radical Reaction Rate Coefficients for Several Isomers and Enantiomers and Their Atmospheric Lifetimes and Global Warming Potentials

机译：甲基全氟庚烯醚（CH_3OC_7F_（13））：几种异构体和对映异构体的测得的OH自由基反应速率系数及其大气寿命和全球变暖潜能

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摘要

Mixtures of methyl-perfluoroheptene-ethers (CH_3OC_7F_(13), MPHEs) are currently in use as replacements for perfluorinated alkanes (PFCs) and poly-ether heat transfer fluids, which are persistent greenhouse gases with lifetimes ＞1000 years. At present, the atmospheric processing and environmental impact from the use of MPHEs is unknown. In this work, rate coefficients at 296 K for the gas-phase reaction of the OH radical with six key isomers (including stereoisomers and enantiomers) of MPHEs used commercially were measured using a relative rate method. Rate coefficients for the six MPHE isomers ranged from ～0.1 to 2.9×10~(-12) cm~3 molecule~(-1) s~(-1) with a strong stereoisomer and -OCH_3 group position dependence; the (E)-stereoisomers with the -OCH_3 group in an α- position relative to the double bond had the greatest reactivity. Rate coefficients measured for the d_3-MPHE isomer analogues showed decreased reactivity consistent with a minor contribution of H atom abstraction from the -OCH_3 group to the overall reactivity. Estimated atmospheric lifetimes for the MPHE isomers range from days to months. Atmospheric lifetimes, radiative efficiencies, and global wanning potentials for these short-lived MPHE isomers were estimated based on the measured OH rate coefficients along with measured and theoretically calculated MPHE infrared absorption spectra. Our results highlight the importance of quantifying the atmospheric impact of individual components in an isomeric mixture.
机译：甲基全氟庚烯醚（CH_3OC_7F_（13），MPHE）的混合物目前被用作全氟烷烃（PFC）和聚醚传热流体的替代品，它们是持久性温室气体，使用寿命＞ 1000年。目前，使用MPHEs对大气的处理和环境影响尚不清楚。在这项工作中，使用相对速率法测量了OH自由基与商用MPHE的六个关键异构体（包括立体异构体和对映异构体）的气相反应在296 K时的速率系数。六种MPHE异构体的速率系数在〜0.1至2.9×10〜（-12）cm〜3分子〜（-1）s〜（-1）范围内，具有很强的立体异构体和-OCH_3基团位置依赖性。 -OCH_3基相对于双键处于α-位的（E）-立体异构体具有最大的反应性。为d_3-MPHE异构体类似物测得的速率系数显示出降低的反应活性，这与从-OCH_3基团夺取H原子对总体反应性的贡献较小有关。 MPHE异构体的估计大气寿命为数天至数月。这些短寿命MPHE异构体的大气寿命，辐射效率和整体减弱电位是根据测得的OH速率系数以及测得的和理论上计算出的MPHE红外吸收光谱估算出来的。我们的结果突出了量化异构混合物中单个成分对大气影响的重要性。

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  • 来源
    《Environmental Science & Technology》 |2014年第9期|4954-4962|共9页
  • 作者

    Aaron M. Jubb; Tomasz Gierczak; Munkhbayar Baasandorj; Robert L. Waterland; James B. Burkholder;

  • 作者单位

    Earth System Research Laboratory, Chemical Sciences Division, National Oceanic and Atmospheric Administration, 325 Broadway, Boulder, Colorado 80305, United States,Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, Colorado 80309, United States;

    Earth System Research Laboratory, Chemical Sciences Division, National Oceanic and Atmospheric Administration, 325 Broadway, Boulder, Colorado 80305, United States,Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, Colorado 80309, United States,Department of Chemistry, Warsaw University, al. Zwirki i Wigury 101, 02-089 Warszawa, Poland;

    Earth System Research Laboratory, Chemical Sciences Division, National Oceanic and Atmospheric Administration, 325 Broadway, Boulder, Colorado 80305, United States,Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, Colorado 80309, United States,Department of Soil, Water, and Climate, University of Minnesota, St. Paul, MN 55108, United States;

    DuPont Central R&D, Wilmington, Delaware 19880, United States;

    Earth System Research Laboratory, Chemical Sciences Division, National Oceanic and Atmospheric Administration, 325 Broadway, Boulder, Colorado 80305, United States;

  • 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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