高污染区域海洋排放对大气化学影响的数值模拟研究

海洋占据了地球表面超过三分之二的面积，是大气中物质的重要来源，可以向大气排放众多气体和颗粒物，可能对大气化学有重要的影响，进而影响全球气候和陆地大气环境。在全球变化以及空气污染快速转变的背景下，理解海洋排放物质的影响对沿海高污染地区空气质量精细管控和区域气候研究等有重要意义。然而，前人在海气物质交换领域的研究主要针对其短期和长期气候平均效应。本研究在此基础上进一步研究海洋排放对区域大气化学产生影响的具体过程，旨在揭示海洋排放对大气环境影响水平、时空演变特征和机理，识别其中的关键物种和要素。

本研究通过对数值模型海洋排放源模块和化学模块的改进，结合过程分析和综合反应速率分析系统性地对不同海洋排放物种、化学反应途径、物理过程的响应进行定量分析，并通过敏感性实验，评估了海洋排放源速率的不确定性影响。基于这些模拟和分析，本研究对海洋排放的大气环境影响进行综合评估：首先研究了海洋排放卤素物质对东亚区域夏季氢氧自由基(OH)浓度影响的机制和特征。其次，在此基础上探索了东亚沿海高污染区域臭氧(O₃)浓度在污染和非污染条件下所受的不同影响及相应途径。最后进行了东亚颗粒物(PM)在不同粒径上对海洋排放的不同响应的研究。

研究结果显示，海洋排放卤素对东亚区域陆地和海洋OH自由基均有重要影响。海洋上OH浓度变化有复杂的正负分布，由海盐气溶胶(SSA)的消光作用和无机碘排放引起的O₃沉降作用等物理过程的负贡献，以及SSA氯化学和无机碘化学的整体正贡献共同确定其具体分布。其中无机碘化学主导了西北太平洋区域的分布特征，在菲律宾海区域出现特殊的负响应极值。这是由于碘化学本身既可以通过消耗O₃来减少OH，又可以加快过氧自由基到OH的转化而增加OH，两者的强弱主要受O₃消耗积累的影响；而在菲律宾海，O₃消耗的积累最明显，因此OH浓度下降最大。

海洋大气碘化学影响OH的过程伴随着大量的O₃消耗，这主导了月平均尺度上O₃浓度的降低；O₃浓度降低幅度有明显的海陆梯度以及污染天和清洁天的区别。与此相反，SSA氯化学虽然对O₃平均值影响有限，但是在高污染区域(以粤港澳大湾区为例)可能对O₃污染产生加重作用。这主要是由于大湾区人为源污染(即高浓度的二氧化氮和O₃及其在夜间反应生成五氧化二氮)使海洋源SSA氯快速活化，生成的硝酰氯气体在光解作用下增加大气氧化性，导致大湾区O₃在污染天的早上增加，幅度可达12 ppbv。虽然污染天碘化学对O₃的消耗贡献也加强，但是由此引起的O₃减少受静稳等气象条件的影响主要集中在海上，无法抵消陆地上氯化学引起的O₃增加。

不同于O₃，陆地PM受到的海洋影响与氧化性关系较小，而是主要通过酸取代反应和粒径再分配来显著减少细颗粒硝酸盐浓度，增加粗颗粒浓度。此外，海洋排放异戊二烯和二甲基硫对PM有一定影响，前者可以降低华北平原南部的硝酸盐浓度，后者则增加大部分区域的硫酸盐浓度。

研究结果揭示了海洋自然排放源能够显著影响东亚夏季大气氧化性以及加重高污染区域的臭氧污染水平，这些影响与海洋排放源的排放速率关系较小，而主要受海‒陆‒气物理化学耦合的相互作用的影响。

The ocean occupies more than two thirds of the earth's surface and is one of the most important sources of atmospheric components. It can emit many gases and particulate matters into the atmosphere, which may have an important impact on atmospheric chemistry, thereby affecting the global climate and terrestrial atmospheric environment. Under the circumstances of global changes and rapid changes in air pollution, understanding the impact of marine emissions is of great significance. Previous studies mainly focused on the average effects of marine emissions, relevant to climate impacts. This study steps further, focusing on the specific processes of the impact of marine emissions on regional atmospheric environment, in order to understand the spatiotemporal evolution of the impact, and to identify the dominant species and key processes.

In this study, we modified some modules of marine emission and chemistry in numerical models, and conducted process analysis as well as sensitivity simulations with different emission rates, in order to systematically quantify the atmospheric responses to different marine-emitted species, chemical pathways, and physical processes. Based on these simulations and analyses, this study conducts a comprehensive evaluation of the impact of marine emissions on the atmospheric environment: First, the mechanisms and characteristics of the impacts of marine-emitted halogens on summertime OH concentrations in East Asia were studied. On this basis, different responses of O₃ concentration, on polluted and clean days, to marine emissions in high polluted coastal areas were explored. Moreover, different impacts of marine emissions on particulate matters with different sizes were also investigated.

The results show that marine halogens have an important impact on OH concentration in East Asia. The change of OH concentration has a complicated positive and negative distribution, which is determined mainly by physical (negative) and chemical (positive in general) processes related to SSA and inorganic iodine emissions. Among these processes, iodine chemistry dominates the distribution characteristics of the distribution in the western Pacific Ocean, showing a special negative extremum in the Philippine Sea. This is because iodine chemistry itself may reduce OH by consuming O₃, and increase OH by accelerating the conversion of peroxyl radicals to OH. The relative strength of both is mainly affected by the accumulation of O₃ depletion. In the Philippine Sea, the accumulation of O₃ depletion is most pronounced and hence the drop in OH concentration is the largest.

Iodine chemistry consumes a large amount of O₃, dominating the decrease of O₃ on a monthly average scale; the decrease of average O₃ has an obvious onshore gradient and a difference between polluted days and clean days. In contrast, although SSA chlorine chemistry has a limited impact on the average O₃, it may deteriorate O₃ pollution in high polluted areas (take the Guangdong-Hong Kong-Macao Greater Bay Area, the GBA for short, as an example). This is mainly due to the high concentration of pollutants from anthropogenic sources (i.e., nitrogen dioxide and O₃ and their product at night), which rapidly activate SSA chloride, and generate nitroxyl chloride gas that can increase atmospheric oxidation capacity (AOC) through photolysis. The increased AOC leads to an increase of O₃ in the GBA in the morning of polluted days, with a magnitude of up to 12 ppbv. Although the consumption of O₃ by iodine chemistry is also enhanced on polluted days, the resultant O₃ depletion is mainly concentrated over ocean and cannot be transported inland efficiently due to meteorological conditions.

Different from O₃, the influence on PM is less related to AOC, but mainly through acid displacement and size redistribution effect that significantly reduce the concentration of fine nitrate and increase the concentration of coarse particle. In addition, marine-emitted isoprene and dimethyl sulfide have some effects on PM. The former can decrease nitrate in the southern part of the North China Plain, while the latter can increase sulfate in most areas.

The results of the study reveal that natural marine emissions can significantly affect the summertime AOC in East Asia and deteriorate the ozone pollution in high polluted areas. These effects are less related to the emission rates, but mainly related to the sea-land-atmosphere coupled physical and chemical interactions.

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