Effects of boundary layer variations on physicochemical characteristics of aerosols in mid-low-altitude regions

Sci Total Environ. 2023 Dec 15:904:166849. doi: 10.1016/j.scitotenv.2023.166849. Epub 2023 Sep 9.

Abstract

Variations in the height of the boundary layer have a critical impact on the vertical transport of near-surface aerosols. Variations can affect the interactions between aerosols and clouds/fog by altering the scattering and absorption of solar radiation, significantly changing radiative forcing, convective precipitation, and regional climate. In this study, we simultaneously monitored air pollution and meteorological factors in a flat urban area (YunTech site, 50 m asl) and its peripheral mountainous region (MeiShan site, 980 m asl), analyzed the characteristics of pollutants under different atmospheric conditions, and explored the differences in the chemical reaction mechanisms of aerosols at various altitudes, aiming to clarify the evolution of the boundary layer in urban and suburban areas and its impact on the transport of pollutants. The results show that even without anthropogenic emissions, urban ground-level pollutants could be transported to peripheral mountainous areas through boundary layer height variations and local circulations, such as mountain-valley breezes. The PM2.5 concentration was higher at the urban site (average 31.14 ± 14.82μgm-3) and could be transported aloft by valley winds, leading to the gradual accumulation of daytime PM2.5 with an afternoon peak at the mountain site. Moreover, the nitrogen oxidation rate (NOR = [NO3-]/[NO3-] + [NO2]) exhibited clear site variations, the mountain site (average 0.41 ± 0.20) was higher than the urban site (average 0.19 ± 0.07), likely due to the atmospheric environment with thick clouds/fog and strong oxidation capacity in the mountain area. Our study has verified that aerosol characteristics, origins, formation pathways and transport mechanisms at the two measurement sites are significantly different under different conditions, which provides a theoretical basis for future air pollution prevention and regional climate research.

Keywords: Atmospheric oxidation capacity; Cloud/fog; Heterogeneous reaction; Local circulation; Planetary boundary layer.