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首页> 外文期刊>Journal of Geophysical Research. Biogeosciences >A modeling study of the nighttime radical chemistry in the lower continental troposphere 1. Development of a detailed chemical mechanism including nighttime chemistry [Review]
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A modeling study of the nighttime radical chemistry in the lower continental troposphere 1. Development of a detailed chemical mechanism including nighttime chemistry [Review]

机译：对流层低层夜间夜间自由基化学的模型研究1.详细的化学机理的开发，包括夜间化学[综述]

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摘要

We describe a detailed chemical mechanism (140 species, 440 reactions) representing atmospheric chemistry of the lower continental troposphere. We focus on chemical reactions potentially important for nighttime chemistry. The mechanism is based on the methods and concepts proposed by Carter [1990] for the development of the Statewide Air Pollution Research Center (SAPRC) mechanism to reduce the number of species and reactions. Peroxy radical chemistry is represented with chemical operators and secondary VOCs are lumped into a limited number of surrogate species. To account for new experimental data provided since the first formulation of the SAPRC mechanism, the whole set of reactions has been updated. Representation of peroxy radical chemistry has been modified to account for variability of organic peroxy radical-peroxy radical reaction rates. New chemical operators and new secondary species have been added to the mechanism to introduce reactions of alkenes with NOB. Reactions of alkenes with O-3 have been largely revised to represent largest radical yields suggested by recent experimental studies. Chemistry of three biogenic compounds (isoprene, a-pinene and P-pinene) has been included. The mechanism is coupled to a two-layer box model (including anthropogenic and biogenic emissions of VOCs and NO, and dry deposition) in order to represent different chemical environments (from urban to rural cases). Comparisons with the SAPRC-99 mechanism show good agreements especially for high NO, regime. Results from the model are evaluated with typical observed concentrations in the different environmental cases with a special focus on the representation of radical species concentations, For both daytime and nighttime, the calculated OH and peroxy radical concentrations are within the range of available observed values although the model tends to overestimate HO2 concentrations in daytime. At night, OH concentrations are found to vary from 1 to 6x10(6) molecules cm(-3) in the urban environment, 5x10(4) to 2x10(5) molecules cm(-3) in polluted rural environments and 4x10(4) molecules cm-3 in remote environments. [References: 146]
机译：我们描述了代表下部大陆对流层大气化学的详细化学机制（140个物种，440个反应）。我们专注于对夜间化学潜在重要的化学反应。该机制基于Carter [1990]提出的方法和概念，用于发展全州空气污染研究中心（SAPRC）的机制，以减少物种和反应的数量。过氧自由基化学以化学运算符表示，并且次要VOC被混入有限数量的替代物种中。为了说明自从首次提出SAPRC机制以来提供的新实验数据，已更新了整个反应集。过氧自由基化学的表示法已被修改，以说明有机过氧自由基-过氧自由基反应速率的变化。该机理中增加了新的化学操作剂和新的次要物种，以引入烯烃与NOB的反应。烯烃与O-3的反应已被大量修订，以代表最近的实验研究表明最大的自由基收率。包括三种生物化合物（异戊二烯，α-pine烯和P-pine烯）的化学成分。该机制耦合到两层盒模型（包括人为和生物排放的VOC和NO，以及干沉降），以代表不同的化学环境（从城市到农村）。与SAPRC-99机制的比较显示出良好的协议，尤其是对于高NO体制。使用不同环境情况下的典型观测浓度评估模型的结果，并特别着重于自由基种类浓度的表示。对于日间和夜间，计算得出的OH和过氧自由基浓度均在可用的观测值范围内，尽管该模型往往会高估白天的HO2浓度。到了晚上，城市环境中的OH浓度从1到6x10（6）分子cm（-3）变化，在污染的农村环境中从5x10（4）到2x10（5）分子cm（-3）变化，而4x10（4） ）分子cm-3在偏远环境中。 [参考：146]

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