Effects of black carbon and boundary layer interaction on surface ozone in Nanjing, China

作者:Gao, Jinhui; Zhu, Bin*; Xiao, Hui; Kang, Hanqing; Pan, Chen; Wang, Dongdong; Wang, Honglei
来源:Atmospheric Chemistry and Physics, 2018, 18(10): 7081-7094.
DOI:10.5194/acp-18-7081-2018

摘要

As an important solar radiation absorbing aerosol, the effect of black carbon (BC) on surface ozone, via reducing photolysis rate, has been widely discussed by "offline" model studies. However, BC-boundary layer (BL) interactions also influence surface ozone. Using the "online" model simulations and process analysis, we demonstrate the significant impact of BC-BL interaction on surface ozone in Nanjing. The absorbing effect of BC heats the air above the BL and suppresses and delays the development of the BL, which eventually leads to a change in surface ozone via a change in the contributions from chemical and physical processes (photochemistry, vertical mixing and advection). For chemical processes, the suppression of the BL leads to large amounts of ozone precursors being confined below the BL which has an increased effect on ozone chemical production and offsets the decrease caused by the reduction of the photolysis rate, thus enhancing ozone chemical formation from 10:00 to 12:00 LT. Furthermore, changes in physical processes, especially the vertical mixing process, show a more significant influence on surface ozone. The weakened turbulence, caused by the suppressed BL, entrains much less ozone aloft down to the surface. Finally, summing-up the changes in the processes, surface ozone reduces before noon and the maximum reduction reaches 16.4 ppb at 12:00 LT. In the afternoon, the changes in chemical process are small which inconspicuously influence surface ozone. However, change in the vertical mixing process still influences surface ozone significantly. Due to the delayed development of the BL, there are obvious ozone gradients around the top of BL. Therefore, high concentrations of ozone aloft can still be entrained down to the surface which offsets the reduction of surface ozone. Comparing the changes in the processes, the change in vertical mixing plays the most important role in impacting surface ozone. Our results highlight the great impacts BC-BL interactions have on surface ozone by influencing the ozone contribution from physical process. This suggests that more attention should be paid to the mechanism of aerosol-BL interactions when controlling ozone pollution.