Spatial variability of air pollutants in a megacity characterized by mobile measurements

Abstract

Abstract. Characterization of the spatial distributions of air pollutants on an intracity scale is important for understanding local sources, secondary formation, and human exposure. In this study, we conducted in situ mobile measurements for the chemical composition of fine particles, volatile organic compounds (VOCs), oxygenated VOCs (OVOCs), and common gas pollutants in winter in the megacity of Beijing. The spatial patterns of these pollutants under different pollution conditions were investigated. During the non-haze days all pollutants showed significant spatial variability. Large spatial variations of secondary species including OVOCs and secondary aerosol species highlight the chemical heterogeneity. In particular, the inorganic chemical composition of fine particles varied greatly on the 65 km urban highway, suggesting a wide range of particle neutralization in the megacity of Beijing. Localized sources such as vehicle, cooking, and industrial emissions led to hot spots and nonuniform distributions of primary pollutants in the city. The spatial heterogeneity of air pollutants under less polluted conditions calls for a future need of using fine-resolution models to evaluate human exposure and to develop pollution control strategies. During the haze day the spatial variabilities of secondary gaseous and particulate pollutants were largely reduced, explained by both the elevated urban background of the polluted air mass and the enhanced secondary formation by elevated precursor concentrations and heterogeneous or aqueous pathways. Although localized primary emissions were accumulated under stagnant haze conditions, the chemical composition of fine particles became relatively homogeneous because of the predominant secondary contributions. A uniform spatial pattern of particle neutralization was observed. The concentrations of hydrocarbons and less oxygenated OVOCs showed good positive spatiotemporal correlations during the haze day, while the concentrations of more oxygenated OVOCs showed good positive correlations among themselves but moderate negative correlations with the concentrations of hydrocarbons, less oxygenated OVOCs, and aerosol species. Our results indicate a spatial chemical homogeneity on the megacity scale to promote efficient secondary organic aerosol (SOA) production under haze conditions.