Secondary aerosol formation and its linkage with synoptic conditions during winter haze pollution over eastern China

摘要

Eastern China has been facing severe winter haze pollution due mainly to secondary aerosol. Existing studies have suggested that stagnant weather or fast chemical production led to frequent haze in this region. However, few works focus on the linkage between secondary production of sulfate, nitrate, and ammonium (SNA) and synoptic conditions, and their joint contribution to PM_(2.5). In this study, by combining in-situ measurements on meteorology and aerosol chemical composition at three main cities together with a regional model with improved diagnose scheme, we investigated the chemical formation and accumulation of main secondary composition, i.e. SNA under typical synoptic conditions. It is indicated that SNA did play a vital role in haze pollution across eastern China, contributing more than 40% to PM_(2.5) mass concentration. As most fast developing region, the Yangtze River Delta (YRD) was slightly polluted during stable weather with local chemical production accounting for 61% SNA pollution. While under the influence of cold front, the pollution was aggravated and advection transport became the predominant contributive process (85%). Nevertheless, the chemical production of SNA was notably enhanced due to the uplift of air pollutant and elevated humidity ahead of the cold front which then facilitated the heterogeneous and aqueous-phase oxidation of precursors. We also found the substantial difference in the phase equilibrium of nitrate over the land surface and ocean due to changes in temperature, ammonia availability and dry deposition. This study highlights the close link between synoptic weather and chemical production, and the resultant vertical and spatial heterogeneity of pollution.