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Ship-plume sulfur chemistry: ITCT 2K2 case study

机译：船用硫磺化学：ITCT 2K2案例研究

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摘要

The ship-plume sulfur chemistry was investigated for the ITCT 2K2 (Intercontinental Transport and Chemical Transformation 2002) ship-plume experiment, using the ship-plume photochemical/dynamic model developed in this study. In order to evaluate the performance of the model, the model-predicted mixing ratios of SO_2 and H_2SO_4 were compared with those observed. From these comparisons, it was found that the model-predicted levels were in reasonable agreements with those observed (0.566.5). According to the multiple ship-plume photochemical/dynamic model simulations, the estimated τ_(SO_2)~(eq) over the entire ship plumes ranged from 10.32 to 14.32 h under moderately stable (E) to stable (F) MBL conditions. These values were clearly shorter than the background SO_2 lifetime (τ_(SO_2)~b) of 15.18-23.20 h. In contrast, τ_(SO_2)~(eq) was estimated to be 0.33 h when the pH_(ss) remained at -8.0 (a rather unlikely case). In addition, the SO_2 loss budget was further analyzed to estimate the influences of the two main factors on the ship-plume sulfur chemistry. The changes in the loss budget with pH_(ss) clearly showed a shift in the dominant SO_2 loss processes from heterogeneous SO_2 conversion (when pH_(ss)>~6.5) to the gas-phase oxidation of SO_2 by OH (when pH_(ss)<-6.5).
机译：使用本研究开发的舰船光化学/动力学模型，对舰船硫化学进行了ITCT 2K2（洲际运输和化学转化2002）舰船实验的研究。为了评估模型的性能，将模型预测的SO_2和H_2SO_4的混合比与观察到的混合比进行了比较。从这些比较中发现，当海盐颗粒的pH（pH_（ss））≤〜6.5时，模型预测的水平与观察到的水平合理一致（0.56 6.5）反应时发生的。根据多次船羽光化学/动力学模型模拟，在中等（E）至稳定（F）MBL条件下，整个船羽的估计τ_（SO_2）〜（eq）范围为10.32至14.32h。这些值明显短于15.18-23.20 h的背景SO_2寿命（τ_（SO_2）〜b）。相反，当pH_（ss）保持在-8.0时，τ_（SO_2）〜（eq）估计为0.33 h（一种不太可能的情况）。此外，进一步分析了SO_2的损失预算，以评估这两个主要因素对船用硫磺化学的影响。损失预算随pH_（ss）的变化清楚地表明，主要的SO_2损失过程已从异质SO_2转化（当pH_（ss）>〜6.5时）转变为OH氧化SO_2时（当pH_（ss）时）。 ）-6.5）。

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