Abstract. More size-resolved chemical information is needed before the physicochemical characteristics and sources of airborne particles can be understood, but this information remains unavailable in most regions of China due to a paucity of measurement data. In this study, we report a one-year observation of various chemical species in size-segregated particle samples collected in urban Beijing, a mega city that experiences severe haze episodes. In addition to fine particles, the measured particle size distributions showed high concentrations of coarse particles during the haze periods. The abundance and chemical compositions of the particles in this study were temporally and spatially variable, with major contributions from organic matter and secondary inorganic aerosols. The contribution of the organic matter to the mass decreased from 37.9 to 33.1%, whereas the total contribution of SO42−, NO3− and NH4+ increased from 19.1 to 32.3% on non-haze and haze days, respectively. Due to heterogeneous reactions and hygroscopic growth, the peaks in the size distributions of organic carbon, SO42−, NO3−, NH4+, Cl−, K+ and Cu shifted from 0.43–0.65 μm on non-haze days to 0.65–1.1 μm on haze days. Although the size distributions are similar for the heavy metals Pb, Cd and Tl during the observation period, their concentrations increased by a factor of more than 1.5 on haze days compared with non-haze days. We found that NH4+ with a size range of 0.43–0.65 μm, SO42− and NO3− with a size range of 0.65–1.1 μm and Ca2+ with a size range of 5.8–9 μm as well as the meteorological factors of relative humidity and wind speed were responsible for the haze pollution when the visibility was less than 15 km. Source apportionment using positive matrix factorization identified six common sources: secondary inorganic aerosols (26.1% for fine particles vs. 9.5% for coarse particles), coal combustion (19 vs. 23.6%), primary emissions from vehicles (5.9 vs. 8.0%), biomass burning (8.5 vs. 2.9%), industrial pollution (6.3 vs. 8.5%) and mineral dust (16.1 vs. 35.1%). The first four factors were higher on haze days, while the latter factors were higher on non-haze days. The sources generally increased with decreasing size with the exception of mineral dust. However, two peaks were consistently found in the fine and coarse particles. The contributing sources also varied with the wind direction; coal and oil combustion products increased during southern flows, indicating that any mitigation strategy should consider the wind pattern, especially during the haze periods. The findings indicated that the PM2.5-based dataset is insufficient for the Chinese source control policy, and detailed size-resolved information is urgently needed to characterize the important sources in urban regions and better understand severe haze pollution.
The Need to Accurately Define and Measure the Properties of Particles