Secondary organic aerosol (SOA) contributes a significant fraction to aerosol mass and toxicity.Low-volatility organic vapors are critical intermediates connecting the oxidation of volatile organic compounds (VOCs) to SOA formation. However, the direct measurement of intermediate vapors poses a great challenge, further compounded by the difficulty of linking them to specific precursors from a cocktail of complex emission sources in the vast urbanized areas. Here, we present coordinated measurements of low-volatility oxidation products, termed oxygenated organic molecules (OOMs) in three most urbanized regions in China. With a newly-developed analysis methodology, we are able to assign these OOMs to their likely precursors and ultimately connect SOA formation to various VOCs. At all measurement locations, we find similar OOM
Understanding the atmospheric new particle formation (NPF) process within the global range is important for revealing the budget of atmospheric aerosols and their impacts. We investigated the seasonal characteristics of NPF in the urban environment of Beijing. Aerosol size distributions down to ∼1∼1 nm and H 2 SO 4 concentration were measured during 2018-2019.2018-2019. The observed formation rate of 1.5 nm particles (J 1.5 ) is significantly higher than those in the clean environment, e.g., Hyytiala;Hyytiala, whereas the growth rate is relatively lower. Both J 1.5 and NPF frequency in urban Beijing showed a clear seasonal variation with maxima in winter and minima in summer, while the observed growth rates were generally within the same range around the year. We show that ambient temperature is a governing factor driving the seasonal variation of J 1.5 . In contrast, the condensation sink showed no significant seasonal variation during the NPF periods and the daily maximum H 2 SO 4 concentration was slightly higher in summer than that in winter. In all four seasons, condensation of H 2 SO 4 and (H 2 SO 4 ) nn (amine) nn clusters contributes significantly to the growth rates in the sub-3 nm size range, whereas it is less important for the observed growth rates of particles above 3 nm. Therefore, other species are always needed for the growth of larger particles.
PM2.5 during severe winter haze in Beijing, China, has reached levels as high as 880 μg/m3, with sulfur compounds contributing significantly to PM2.5 composition. This sulfur has been traditionally assumed to be sulfate, although atmospheric chemistry models are unable to account for such large sulfate enhancements under dim winter conditions. Using a 1‐D model, we show that well‐characterized but previously overlooked chemistry of aqueous‐phase HCHO and S(IV) in cloud droplets to form a S(IV)‐HCHO adduct, hydroxymethane sulfonate, may explain high particulate sulfur in wintertime Beijing. We also demonstrate in the laboratory that methods of ion chromatography typically used to measure ambient particulates easily misinterpret hydroxymethane sulfonate as sulfate. Our findings suggest that HCHO and not SO2 has been the limiting factor in many haze events in Beijing and that to reduce severe winter pollution in this region, policymakers may need to address HCHO sources such as transportation.
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