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Chemical evolution and dispersion of ship plumes in the remote marine boundary layer: investigation of sulfur chemistry

机译：偏远海洋边界层中船羽的化学演化和扩散：硫化学研究

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In this study a Lagrangain photochemical box model has been used to explore gaseous/heterogeneous sulfur plume chemistry initiated by ship traffic in the MBL. The results indicate that although SO_2 ship emission rates have an impact on the concentration levels of SO_2, there is no evidence of non-linear loss processes in this chemical system. This finding as well as others have demonstrated that the major loss pathway for SO_2 is via heterogeneous loss to sea-salt aerosol. This loss rate, however, can be greatly influenced by the MET condition selected for the MBL. For example, the "stable" MET condition leads to the maximum loss rate, whereas the "unstable" condition gives the minimum value. In the case of H_2SO_4(g), the "stable" MET condition provides both the highest SO_2 and OH concentrations, and hence, the formation rate is also maximized. It was found that increases in aerosol surface area (i.e., heterogeneous loss) as well as shifts to higher latitudes (e.g., lower T and higher O_3 levels) tended to increase the rate of loss of SO_2 due to enhancements in the rates of heterogeneous chemistry. However, the single largest factor that influenced the rate of SO_2 loss was the presence of BL clouds where oxidation via scavenged H_2O_2 was the dominant process. Quite significant also was the finding that photochemical processes, because of their production of OH, O_3, and H_2O_2, are strongly coupled to SO_2 sea-salt heterogeneous reactions, cloud heterogeneous reactions, and gas-phase reactions to form H_2SO_4. Not surprisingly, therefore, model predictions of the rate of formation of new particles within ship plumes were found to be quite dependent on the intensity of photochemistry.
机译：在这项研究中，拉格朗日光化学箱模型已用于探索MBL中船舶交通引发的气态/非均质硫羽化学。结果表明，尽管SO_2的船舶排放速率对SO_2的浓度水平有影响，但没有证据表明该化学系统中存在非线性损失过程。这一发现以及其他发现表明，SO_2的主要损失途径是通过向海盐气溶胶的非均质损失。但是，此丢失率可能会受到为MBL选择的MET条件的很大影响。例如，“稳定” MET条件导致最大损失率，而“不稳定”条件给出最小值。在H_2SO_4（g）的情况下，“稳定”的MET条件同时提供最高的SO_2和OH浓度，因此，形成速率也最大化。已经发现，由于异质化学速率的提高，气溶胶表面积的增加（即，非均质的损失）以及向较高纬度（例如，较低的T和较高的O_3水平）的转移倾向于增加SO_2的损失速率。 。然而，影响SO_2损失速率的最大因素是BL云的存在，其中通过清除的H_2O_2氧化是主要过程。同样非常重要的发现是，由于光化学过程产生OH，O_3和H_2O_2，它们与SO_2海盐异质反应，云异质反应和气相反应强烈结合，形成H_2SO_4。因此，毫不奇怪，发现船羽内新颗粒形成速率的模型预测完全取决于光化学强度。

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