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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Reaction of oleic acid particles with NO3 radicals: Products, mechanism, and implications for radical-initiated organic aerosol oxidation
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Reaction of oleic acid particles with NO3 radicals: Products, mechanism, and implications for radical-initiated organic aerosol oxidation

机译：油酸颗粒与NO3自由基的反应：自由基引发的有机气溶胶氧化的产物，机理和意义

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摘要

The heterogeneous reaction of liquid oleic acid aerosol particles with NO3 radicals in the presence of NO2, N2O5, and O-2 was investigated in an environmental chamber using a combination of on-line and off-line mass spectrometric techniques. The results indicate that the major reaction products, which are all carboxylic acids, consist of hydroxy nitrates, carbonyl nitrates, dinitrates, hydroxydinitrates, and possibly more highly nitrated products. The key intermediate in the reaction is the nitrooxyalkylperoxy radical, which is formed by the addition of NO3 to the carbon-carbon double bond and subsequent addition Of O-2. The nitrooxyalkylperoxy radicals undergo self-reactions to form hydroxy nitrates and carbonyl nitrates, and may also react with NO2 to form nitrooxy peroxynitrates. The latter compounds are unstable and decompose to carbonyl nitrates and dinitrates. It is noteworthy that in this reaction nitrooxyalkoxy radicals appear not to be formed, as indicated by the absence of the expected products of decomposition or isomerization of these species. This is different from gas-phase alkene-NO3 reactions, in which a large fraction of the products are formed through these pathways. The results may indicate that, for liquid organic aerosol particles in low NOx environments, the major products of the radical-initiated oxidation (including by OH radicals) of unsaturated and saturated organic compounds will be substituted forms of the parent compound rather than smaller decomposition products. These compounds will remain in the particle and can potentially enhance particle hygroscopicity and the ability of particles to act as cloud condensation nuclei.
机译：在NO2，N2O5和O-2存在下，使用在线和离线质谱技术相结合，研究了液体油酸气溶胶颗粒与NO3自由基的异质反应。结果表明，全部为羧酸的主要反应产物由羟基硝酸盐，羰基硝酸盐，二硝酸盐，羟基短酸盐以及可能更高硝酸化的产物组成。反应中的关键中间体是硝基氧烷基过氧自由基，它是通过将NO3加至碳-碳双键并随后加成O-2形成的。硝基氧烷基过氧自由基经过自反应形成羟基硝酸盐和羰基硝酸盐，并且还可能与NO2反应形成硝基氧过氧硝酸盐。后面的化合物不稳定，并分解为羰基硝酸盐和二硝酸盐。值得注意的是，在该反应中似乎没有形成硝基氧基烷氧基，如不存在这些物质的分解或异构化的预期产物所表明的那样。这与气相烯烃-NO3反应不同，在气相烯烃-NO3反应中，大部分产物是通过这些途径形成的。结果可能表明，对于低NOx环境中的液态有机气溶胶颗粒，不饱和和饱和有机化合物的自由基引发氧化（包括通过OH自由基）的主要产物将是母体化合物的取代形式，而不是较小的分解产物。这些化合物将保留在颗粒中，并可能增强颗粒的吸湿性和颗粒充当云凝结核的能力。

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