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    气溶胶影响边界层臭氧光化学过程的观测和模拟

    Study on the Effects of Aerosols on Ozone Photochemical Processes in the Boundary Layer Based on Observation and Simulation

    • 摘要: 基于2018—2022年南京市5次短期边界层强化探空数据,结合以观测资料为基础的系列模型,讨论了不同类型气溶胶对边界层臭氧光化学过程影响的作用机制。观测结果表明:边界层内吸收性气溶胶与臭氧浓度呈负相关,对臭氧的光化学生成起抑制作用;散射性气溶胶与臭氧浓度在边界层上方呈正相关,对臭氧光化学生成起促进作用。污染天边界层顶臭氧体积分数和向下短波辐射出现突增现象,每百米变化分别为4.8×10-9和20.6 W/m2,而清洁天仅为0.8×10-9和6.6 W/m2。模拟研究发现,吸收性气溶胶削弱整层向上短波辐射,近地层最大可削弱4.4 W/m2,并降低整层二氧化氮光解率(JNO2),进而抑制臭氧生成。散射性气溶胶可增强边界层上部向上短波辐射,最高可达4.5 W/m2,并提高上部JNO2,进而刺激边界层上部臭氧的光化学生成。吸收性和散射性气溶胶的浓度配比不会改变气溶胶类型对臭氧光化学生成的作用机制。

       

      Abstract: Based on the data of five short-term boundary layer vertical observations in Nanjing from 2018 to 2022,combined with a series of observation-based models,the effect of different types of aerosols on the photochemical processes of ozone (O3) in the boundary layer was discussed in this study.The observed results show that absorbing aerosols in the boundary layer are negatively correlated with the ozone concentrations,inhibiting ozone photochemical formation.Scattering aerosols are positively correlated with ozone concentrations above the boundary layer,promoting ozone formation.The ozone volume fraction and downward shortwave radiation at the top of the boundary layer increased abruptly on polluted days,and the changes were 4.8×10-9 and 20.6 W/m2 per 100 meters,respectively,while the changes were only 0.8×10-9 and 6.6 W/m2 on clean days.The simulation results show that the absorbing aerosols reduce upward shortwave radiation throughout the whole layer,with a maximum reduction of 4.4 W/m2 near the surface,and then reduce the photolysis rate of nitrogen dioxide (JNO2) across the column,thereby inhibiting ozone formation.Scattering aerosols enhance upward shortwave radiation up to 4.5 W/m2 in the upper layer,and increase JNO2,thereby stimulating ozone photochemical generation in the upper boundary layer.The concentration ratio of absorbing to scattering aerosols does not change the mechanism of aerosol type on ozone photochemical formation.

       

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