Sulfate aerosols exert profound impacts on human and ecosystem health, weather, and climate, but their formation mechanism remains uncertain. Atmospheric models consistently underpredict sulfate levels under diverse environmental conditions. From atmospheric measurements in two Chinese megacities and complementary laboratory experiments, we show that the aqueous oxidation of SO 2 by NO 2 is key to efficient sulfate formation but is only feasible under two atmospheric conditions: on fine aerosols with high relative humidity and NH 3 neutralization or under cloud conditions. Under polluted environments, this SO 2 oxidation process leads to large sulfate production rates and promotes formation of nitrate and organic matter on aqueous particles, exacerbating severe haze development. Effective haze mitigation is achievable by intervening in the sulfate formation process with enforced NH 3 and NO 2 control measures. In addition to explaining the polluted episodes currently occurring in China and during the 1952 London Fog, this sulfate production mechanism is widespread, and our results suggest a way to tackle this growing problem in China and much of the developing world.sulfate aerosol | severe haze | pollution | human health | climate

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1] Total suspended particles (TSP) were collected at the summit of Mt. Tai (1534 m above sea level) on a daytime and nighttime basis during a summertime campaign (May-June 2006) and were characterized for organic molecular compositions using solvent extraction/derivatization and gas chromatography/mass spectrometry technique. The n-Alkanes, fatty acids, fatty alcohols, sugars, glycerol and polyacids, and phthalate esters were found as major organic compound classes, whereas lignin and resin products, sterols, aromatic acids, hopanes, and polycyclic aromatic hydrocarbons (PAHs) were detected as minor classes. Sugars (49.8-2115 ng m À3 , average 640 ng m À3 in daytime; 18.1-4348 ng m À3 , 799 ng m À3 in nighttime) were found to be the dominant compound class. Levoglucosan, a specific cellulose pyrolysis product, was detected as the most abundant single compound, followed by C 28 fatty alcohol, diisobutyl and di-n-butyl phthalates, C 29 n-alkane, C 16 and C 28 fatty acids, and malic acid. By grouping organic compounds based on their sources, we found that emission of terrestrial plant waxes was the most significant source (30-34%) of the TSP, followed by biomass burning products (25-27%) (e.g., levoglucosan and lignin and resin products), soil resuspension (15-18%) due to agricultural activities, secondary oxidation products (8-10%), plastic emission (3-10%), marine/microbial sources (6%), and urban/industrial emissions from fossil fuel use (4%). However, low molecular weight dicarboxylic acids (such as oxalic acid) of photochemical origin were not included in this study. Malic acid was found to be much higher than those reported in the ground level, suggesting an enhanced photochemical production in the free troposphere over mountain areas. Temporal variations of biomass burning tracers (e.g., levoglucosan, galactosan, mannosan) and some higher plant wax derived compound classes suggested that there were two major (E1 and E2) and one minor (E3) biomass-burning events during this campaign. Most of the compound classes showed higher concentrations in nighttime samples when organic aerosols can be long-range transported from different source regions to the summit of Mt. Tai above the planetary boundary layer (PBL). This study also demonstrates that the free troposphere over Mt. Tai is heavily influenced by field burning of agricultural wastes such as wheat straws in the North China Plain during the harvest season in early summer.

Organic aerosols were studied at the molecular level in 14 coastal and inland mega-cities in China during winter and summer 2003. They are characterized by the abundant presence of n-alkanes (annual average, 340 ng m(-3)), fatty acids (769 ng m(-3)), sugars (412 ng m(-3)), and phthalates (387 ng m(-3)). In contrast, fatty alcohols, polyols/polyacids, lignin and resin products, sterols, polycyclic aromatic hydrocarbons (PAHs), and hopanes were detected as relatively minor components. n-Alkanes show a weak odd/even carbon predominance (CPI = 1.1) and PAHs show a predominance of benzo(b)fluoranthene, suggesting a serious contribution from fossil fuel (mainly coal) combustion. Their concentrations (except for phthalates and polyols/polyacids) were 2-15 times higher in winter than summer due to a significant usage of coal burning and an enhancement of atmospheric inversion layers. Phthalates were found to be more abundant in summer than winter, probably due to enhanced vaporization from plastics followed by adsorptive deposition on the pre-existing particles. Concentrations of total quantified compounds are extremely high (approximately 10 microg m(-3)) in the midwest (Chongqing and Xi'an) where active industrialization/urbanization is going on. This study shows that concentrations of the compounds detected are 1-3 orders of magnitude higher than those reported from developed countries.

Although regional haze adversely affects human health and possibly counteracts global warming from increasing levels of greenhouse gases, the formation and radiative forcing of regional haze on climate remain uncertain. By combining field measurements, laboratory experiments, and model simulations, we show a remarkable role of black carbon (BC) particles in driving the formation and trend of regional haze. Our analysis of long-term measurements in China indicates declined frequency of heavy haze events along with significantly reduced SO2, but negligibly alleviated haze severity. Also, no improving trend exists for moderate haze events. Our complementary laboratory experiments demonstrate that SO2 oxidation is efficiently catalyzed on BC particles in the presence of NO2 and NH3, even at low SO2 and intermediate relative humidity levels. Inclusion of the BC reaction accounts for about 90–100% and 30–50% of the sulfate production during moderate and heavy haze events, respectively. Calculations using a radiative transfer model and accounting for the sulfate formation on BC yield an invariant radiative forcing of nearly zero W m−2 on the top of the atmosphere throughout haze development, indicating small net climatic cooling/warming but large surface cooling, atmospheric heating, and air stagnation. This BC catalytic chemistry facilitates haze development and explains the observed trends of regional haze in China. Our results imply that reduction of SO2 alone is insufficient in mitigating haze occurrence and highlight the necessity of accurate representation of the BC chemical and radiative properties in predicting the formation and assessing the impacts of regional haze.

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In this study, 121 daily PM_2.5 (aerosol particle with aerodynamic diameter less than 2.5 μm) samples were collected from an urban site in Beijing in four months between April 2009 and January 2010 representing the four seasons. The samples were determined for various compositions, including elements, ions, and organic/elemental carbon. Various approaches, such as chemical mass balance, positive matrix factorization (PMF), trajectory clustering, and potential source contribution function (PSCF), were employed for characterizing aerosol speciation, identifying likely sources, and apportioning contributions from each likely source. Our results have shown distinctive seasonalities for various aerosol speciations associated with PM_2.5 in Beijing. Soil dust waxes in the spring and wanes in the summer. Regarding the secondary aerosol components, inorganic and organic species may behave in different manners. The former preferentially forms in the hot and humid summer via photochemical reactions, although their precursor gases, such as SO₂ and NO_x, are emitted much more in winter. The latter seems to favorably form in the cold and dry winter. Synoptic meteorological and climate conditions can overwhelm the emission pattern in the formation of secondary aerosols. The PMF model identified six main sources: soil dust, coal combustion, biomass burning, traffic and waste incineration emission, industrial pollution, and secondary inorganic aerosol. Each of these sources has an annual mean contribution of 16, 14, 13, 3, 28, and 26%, respectively, to PM_2.5. However, the relative contributions of these identified sources significantly vary with changing seasons. The results of trajectory clustering and the PSCF method demonstrated that regional sources could be crucial contributors to PM pollution in Beijing. In conclusion, we have unraveled some complex aspects of the pollution sources and formation processes of PM_2.5 in Beijing. To our knowledge, this study is the first systematical study that comprehensively explores the chemical characterizations and source apportionments of PM_2.5 aerosol speciation in Beijing by applying multiple approaches based on a completely seasonal perspective

Microplastics in the air have gradually attracted our attention in recent years; however, temporal and spatial trends of microplastics in indoor air are rarely discussed. In the present study, we tracked microplastic fallout in a dormitory, an office, and a corridor on both workdays and weekends for three months. In addition, an air conditioner was used to understand airflow influence on microplastic resuspension in the dorm. Among the three sampling sites, the highest average microplastic abundance appeared in the dormitory (9.9 × 103 MPs/m2/d), followed by the office (1.8 × 103 MPs/m2/d) and the corridor (1.5 × 103 MPs/m2/d). In the dormitory, the average MP abundance on weekends (1.4 × 104 MPs/m2/d) was approximately three times of that on weekdays (5.8 × 103 MPs/m2/d). In the office; however, the abundance on weekends (1.2 × 103 MPs/m2/d) was 50% of that on weekdays (2.4 × 103 MPs/m2/d). Microplastic fallout existed mostly in the form of fibers and showed similar polymer compositions to the textile products used in indoor environments. The airflow tests using an air conditioner suggested that airflow turbulence increased resuspension of microplastics. Taken together, we conclude that indoor environments are prone to serious microplastic pollution, but microplastic level varies greatly due to different characteristics of indoor setting. Our results also indicate that textile quantity is one of the main factors affecting microplastic abundance in indoor air, whereas air conditioner-induced airflow turbulence can cause microplastic migration in indoor environments.