Abstract
The atmospheric aerosol particles have a potential heavy burden on environment, climate, and human health, which were closely related to the surface physicochemical properties. Time-of-flight secondary ion mass spectrometry (TOF-SIMS) technique is a powerful tool to obtain detailed surface chemical information since it has high surface sensitivity for both elements and molecular ions, and high mass resolution. In this work, size-fractioned aerosol particles in the range of 0.43–10 µm during a severe haze episode in Beijing were analyzed by TOF-SIMS, the variation characteristics of chemical species corresponding to particle size and air pollution level was investigated by the normalization of secondary ion intensities, the possible sources were identified through principal component analysis (PCA), and the influence of meteorological factors and air mass transmission were also investigated. The study results showed that the surface chemical components of PM2.5 were more complicated during haze episode than on clean days. A total of 17 organic and inorganic species were detected, including crustal elements, heavy metals, sulfate, nitrate, siliceous compounds, hydrocarbons, oxygen-containing organics, and nitrogen-containing organics. In general, the particle surface mainly contained crustal elements, hydrocarbons, and carbon-containing inorganics. Organic and secondary ions significantly increased in heavy-polluted days, indicating the aging process of particles. Inorganic compounds had a higher percentage in coarse mode, while organic compounds were higher in accumulation mode. PCA results indicated that urban aerosol during this haze episode mainly came from vehicle emissions (24.7%), coal-fired combustion (22.4%), organic aerosol (19.3%), and dust resuspension (19.6%). The northern air mass could facilitate the dilution of air pollutants with the surface secondary formed components of particles significantly decreased.
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