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Explicit modeling of volatile organic compounds partitioning in the atmospheric aqueous phase

机译:大气水相中挥发性有机化合物分配的显式建模

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摘要

The gas phase oxidation of organic species is a multigenerational process involving a large number of secondary compounds. Most secondary organic species are water-soluble multifunctional oxygenated molecules. The fully explicit chemical mechanism GECKO-A (Generator of Explicit Chemistry and Kinetics of Organics in the Atmosphere) is used to describe the oxidation of organics in the gas phase and their mass transfer to the aqueous phase. The oxidation of three hydrocarbons of atmospheric interest (isoprene, octane and α-pinene) is investigated for various NOx conditions. The simulated oxidative trajectories are examined in a new two dimensional space defined by the mean oxidation state and the solubility. The amount of dissolved organic matter was found to be very low (yield less than 2% on carbon atom basis) under a water content typical of deliquescent aerosols. For cloud water content, 50% (isoprene oxidation) to 70% (octane oxidation) of the carbon atoms are found in the aqueous phase after the removal of the parent hydrocarbons for low NOx conditions. For high NOx conditions, this ratio is only 5% in the isoprene oxidation case, but remains large for α-pinene and octane oxidation cases (40% and 60%, respectively). Although the model does not yet include chemical reactions in the aqueous phase, much of this dissolved organic matter should be processed in cloud drops and modify both oxidation rates and the speciation of organic species.
机译:有机物质的气相氧化是涉及大量二级化合物的多粒程过程。大多数次级有机物是水溶性多官能含氧分子。使用完全明确的化学机制壁虎-A(大气中有机物的显式化学和有机动力学)来描述气相中有机物的氧化及其对水相的传质。研究了三种富含烃(异戊二烯,辛烷值和α-突烯)的三种烃用于各种NOx条件。模拟氧化轨迹在由平均氧化状态和溶解度限定的新的二维空间中检查。在典型的潮热气溶胶的含水含量下,发现溶解有机物的量非常低(碳原子基于碳原子的产量小于2%)。对于云含水量,在除去母体烃的水相中,在母体烃的水相中发现50%(异戊二烯氧化)至70%(辛烷氧化)以进行母体烃,用于低NOx条件。对于高NOx条件,该比例在异戊二烯氧化壳体中仅为5%,但对于α-Pine烯和辛烷氧化案例仍然很大(分别为40%和60%)。虽然该模型尚未包括水相中的化学反应,但大部分溶解的有机物质应在云下处理,并改变氧化率和有机物种的形态。

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