Highly time-resolved in situ measurements of airborne particles were conducted at Mt. Yulong (3410 m above sea level) on the southeastern edge of the Tibetan Plateau in China from 22 March to 14 April 2015. The detailed chemical composition was measured by a high-resolution time-of-flight aerosol mass spectrometer together with other online instruments. The average mass concentration of the submicron particles (PM1) was 5.7 +/- 5.4 mu g m(-3) during the field campaign, ranging from 0.1 up to 33.3 mu g m(-3). Organic aerosol (OA) was the dominant component in PM1, with a fraction of 68 %. Three OA factors, i.e., biomass burning organic aerosol (BBOA), biomass-burning-influenced oxygenated organic aerosol (OOA-BB) and oxygenated organic aerosol (OOA), were resolved using positive matrix factorization analysis. The two oxygenated OA factors accounted for 87% of the total OA mass. Three biomass burning events were identified by examining the enhancement of black carbon concentrations and the f(60) (the ratio of the signal at m/z 60 from the mass spectrum to the total signal of OA). Back trajectories of air masses and satellite fire map data were integrated to identify the biomass burning locations and pollutant transport. The western air masses from South Asia with active biomass burning activities transported large amounts of air pollutants, resulting in elevated organic concentrations up to 4-fold higher than those of the background conditions. This study at Mt. Yulong characterizes the tropospheric background aerosols of the Tibetan Plateau during pre-monsoon season and provides clear evidence that the southeastern edge of the Tibetan Plateau was affected by the transport of anthropogenic aerosols from South Asia.

The heterogeneous hydrolysis of dinitrogen pentoxide (N2O5) is important to understanding the formation of particulate nitrate (pNO(3)(-)). Measurements of N2O5 in the surface layer taken at an urban site in Beijing are presented here. N2O5 was observed with large day-to-day variability. High N2O5 concentrations were determined during pollution episodes with the co-presence of large aerosol loads. The maximum value was 1.3 ppbv (5 s average), associated with an air mass characterized by a high level of O-3. N2O5 uptake coefficients were estimated to be in the range of 0.025-0.072 using the steady-state lifetime method. As a consequence, the nocturnal pNO(3)(-) formation potential by N2O5 heterogeneous uptake was calculated to be 24-85 mu g m(-3) per night and, on average, 57 mu g m(-3) during days with pollution. This was comparable to or even higher than that formed by the partitioning of HNO3. The results highlight that N2O5 heterogeneous hydrolysis is vital in pNO(3)(-) formation in Beijing.

The molecular composition of humic-like[GRAPHIC]substances (HULIS) in different aerosol samples was analyzed using an ultrahigh-resolution mass spectrometer to investigate the influence of biomass burning on ambient aerosol composition. HULIS in background aerosols were characterized with numerous molecular formulas similar to biogenic secondary organic aerosols. The abundance of nitrogen-containing organic compounds (NOC), including nitrogen-containing bases (N-bases) and nitroaromatics, increased dramatically in ambient aerosols affected by crop residue burning in the farm field. The molecular distribution of N-bases in these samples exhibited similar patterns to those observed in smoke particles freshly emitted from lab-controlled burning of straw residues but were significantly different with those observed from wood burning. Signal intensity of the major N-bases correlated well with the atmospheric concentrations of potassium and levoglucosan. These N-bases can serve as molecular markers distinguishing HULIS from crop residue burning with from wood burning. More nitroaromatics were detected in ambient aerosols affected by straw burning than in fresh smoke aerosols, indicating that many of them are formed in secondary oxidation processes as smoke plumes evolve in the atmosphere. This study highlights the significant contribution of crop residue burning to atmospheric NOC. Further study is warranted to evaluate the roles of NOC on climate and human health.

Although organic compounds in marine atmospheric aerosols have significant effects on climate and marine ecosystems, they have rarely been studied, especially in the coastal regions of East China. To assess the origins of the organic aerosols in the East China coastal atmosphere, PM2.5 samples were collected from the atmospheres of the Yellow Sea, the East China Sea, and Changdao Island during the CAPTAIN (Campaign of Air PolluTion At INshore Areas of Eastern China) field campaign in the spring of 2011. The marine atmospheric aerosol samples that were collected were grouped based on the backward trajectories of their air masses. The organic carbon concentrations in the PM2,5 samples from the marine and Changdao Island atmospheres were 5.5 +/- 3.1 mu gC/m(3) and 6.9 +/- 2.4 mu gC/m(3), respectively, which is higher than in other coastal water atmospheres. The concentration of polycyclic aromatic hydrocarbons (PAHs) in the marine atmospheric PM2.5 samples was 17.0 +/- 20.2 ng/m(3), indicating significant continental anthropogenic influences. The influences of fossil fuels and biomass burning on the composition of organic aerosols in the coastal atmosphere of East China were found to be highly dependent on the origins of the air masses. Diesel combustion had a strong impact on air masses from the Yangtze River Delta (YRD), and gasoline emissions had a more significant impact on the "North China" marine atmospheric samples. The "Northeast China" marine atmospheric samples were most impacted by biomass burning. Coal combustion contributed significantly to the compositions of all of the atmospheric samples. The proportions of secondary compounds increased as samples aged in the marine atmosphere indicating that photochemical oxidation occured during transport. Our results quantified ecosystem effects on marine atmospheric aerosols and highlighted the uncertainties that arise when modeling marine atmospheric PM2.5 without considering high spatial resolution source data and meteorological parameters. (C) 2017 Published by Elsevier Ltd.

Rapid economic development and urbanization in China has been concentrated in coastal cities, resulting in haze and photochemical smog issues, especially in the densely-populated Yangtze River Delta. In this study, we explore particulate matter (specifically PM2.5) pollution in a city in Zhejiang Province (Ningbo), chosen to represent a typical, densely-populated urban city with residential and industrial sections. PM2.5 samples were collected at five sites in four seasons from Dec. 2012 to Nov. 2013. The annual average PM2.5 mass concentration was 53.2 +/- 30.4 mu g/m(3), with the highest concentration in winter and lowest in summer. Among the five sites, PM2.5 concentration was highest in an urban residential site and lowest in a suburban site, due to effects of urbanization and the anthropogenic influences. The chemical components of PM2.5 show significant seasonal variation. In addition, secondary transformation was high in Ningbo, with the highest proportion of secondary components found at a suburban site and the lowest at the industrial sites. Ningbo is controlled by five major air masses originating from inland China, from the Bohai Sea, offshore from the southeast, the Yellow Sea, and off the east coast of Korea. The relative contributions of these air masses differ, by season, with the Bohai Sea air mass dominating in winter and spring, the maritime southeast air mass in summer, and the YellowSea and coastal Korean air masses dominating in autumn. The continental air mass is associated with a high PM2.5 concentration, indicating that it is primarily transports primary emissions. In contrast, the concentration ratios among secondary formed pollutants were higher in the maritime air masses, which suggests that sea breezes control temporal and spatial variations of air pollution over coastal cities. (C) 2017 Published by Elsevier B.V.

Gasoline vehicle exhaust is an important contributor to secondary organic aerosol (SOA) formation in urban atmosphere. Fuel composition has a potentially considerable impact on gasoline SOA production, but the link between fuel components and SOA production is still poorly understood. Here, we present chamber experiments to investigate the impacts of gasoline aromatic content on SOA production through chamber oxidation approach. A significant amplification factor of 3-6 for SOA productions from gasoline exhausts is observed as gasoline aromatic content rose from 29 to 37 %. Considerably higher emission of aromatic volatile organic compounds (VOCs) using high-aromatic fuel plays an essential role in the enhancement of SOA production, while semi-volatile organic compounds (e.g., gas-phase PAHs) may also contribute to the higher SOA production. Our findings indicate that gasoline aromatics significantly influence ambient PM2.5 concentration in urban areas and emphasize that more stringent regulation of gasoline aromatic content will lead to considerable benefits for urban air quality.

Particulate organonitrates are formed from volatile organic compounds (VOCs) oxidation by radicals. A portion of semi-volatile gas-phase organonitrates can be incorporate into aerosol by oxidation reactions or portioning, and has been an important component of secondary organic aerosol (SOA). Particulate organonitrates study has become one of the important aspects of atmospheric chemistry. Given the large number and variability of chemical constituents, and possible chemical transformations of organonitrates, such characterization presents a key problem for research. Based on recent research progress on particulate organonitrates, this paper summarizes the formation mechanism and quantification method of particulate organonitrates. Profiting from the application of high time resolution techniques, field measurements has become the major approach of particulate organonitrates study. Thermal dissociation-laser induced fluorescence (TD-LIF) and aerosol mass spectrometers (AMS) have been used to quantify and provide the evolution processes of particulate organonirates. Meanwhile, chemical ionization mass spectrometer(CIMS)allows for the determination of molecular ion composition of organonitrates, promising to become the important direction of study of particulate organonirates in future field measurements. To have a deep insight on precursor and atmospheric chemistry processes of particulate organonirates, future research should focus on the combination of field measurement, modeling simulation and laboratory simulation, and these will also lead to a more comprehensive understanding of formation mechanism of particulate organonirates

New particle formation (NPF) and its subsequent growth plays a key role in air quality and climate change at regional and global scales. Especially under complex air pollution in China, nucleation and growth can be highly efficient, claimed to be a main source of cloud condensation nuclei (CCN) and an important cause of secondary aerosol pollution. Currently, the mechanism of particle formation and growth as well as its environmental effects are still poorly understood. Thereby, fully understanding of the atmospheric nucleation and subsequent growth still presents a big challenge to atmospheric chemistry researches. This study reviews the current results from studies on mechanisms and environmental effects of atmospheric nucleation and growth. We summarize that traditional nucleation theories such as binary nucleation of H2SO4-H2O, ternary nucleation of H2SO4-NH3-H2O, ion-induced nucleation are not capable in explaining new particle formation under complex air pollution, while newly proposed mechanisms such as organic acids and amine induced nucleation were not verified because of technique limitation. We propose that the future researches should focus on identifying the key chemical precursor response for driving nucleation and initial and subsequent growth, and understand the physical and chemical processing of new particle formation and growth. In particularly, application and development of novel techniques, such as APi-TOF-CIMS, PSM, Nano-HTDMA in new particle formation study is very important. Also, future researches should establish whole process tracking on new particle formation, from precursor, nucleation, growth till the environmental effects, by integrating field observation, chamber simulation, and modelling. Currently, the mechanism of highly efficient nucleation and rapid growth taking place under complex air pollution in China is urgently needed to be in-depth studied in order to improve our understanding of regional haze formation. This could be helpful to understand the similarity and difference in the nucleation mechanism between clean and polluted atmospheric environments.

Severe air pollution and its associated health impacts have become one of the major concerns in China. A detailed analysis of PM2.5 chemical compositions is critical for optimizing pollution control measures. In this study, daily 24-h bulk filter samples were collected and analyzed for totally 21 field campaigns at 17 sites in China between 2008 and 2013. The 17 sites were classified into four groups including six urban sites, seven regional sites, two coastal sites in four fast developing regions of China (i.e. Beijing-Tianjin-Hebei region, Yangtze River Delta, Pearl River Delta and Sichuan Basin), and two ship cruise measurements covered the East China Sea and Yellow Sea of China. The high average concentrations of PM2.5 and the occurrences of extreme cases at most sites imply the widespread air pollution in China. Fine particles were largely composed of organic matter and secondary inorganic species at most sites. High correlation between the temporal trends of PM2.5 and secondary species of urban and regional sites highlights the uniformly distributed air pollutants within one region. Secondary inorganic species were the dominant contributors to the high PM2.5 concentration in Northern China. However in Southern China, the relative contributions of different chemical species kept constant as PM2.5 increased. This study provides us a better understanding of the current state of air pollution in diversified Chinese cities. Analysis of chemical signatures of PM2.5 could be a strong support for model validation and emission control strategy. (C) 2016 Elsevier Ltd. All rights reserved.

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 SO2 by NO2 is key to efficient sulfate formation but is only feasible under two atmospheric conditions: on fine aerosols with high relative humidity and NH3 neutralization or under cloud conditions. Under polluted environments, this SO2 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 NH3 and NO2 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.

Chemical composition, morphology, size and mixture of fine particles were measured in a heavy haze and the post-haze air in Beijing in January 2012. With the occurrence of haze, the concentrations of gaseous and particulate pollutants including organics, sulfate, nitrate, and ammonium grew gradually. The hourly averaged PM2.5 concentration increased from 118 mu g m(-3) to 402 mu g m(-3) within 12 h. In contrast, it was less than 10 mu g m(-3) in the post-haze air. Occupying approximately 46% in mass, organics were the major component of PM1 in both the haze and post-haze air.Analysis of individual particles in the size range of 0.2-1.1 mu m revealed that secondary-like particles and soot particles were always the majority, and most soot particles had a core-shell structure. The number ratio of secondary-like particles to soot particles in accumulation mode in the haze air was about 2:1, and that in the post-haze air was 8:1. These results indicate both secondary particle formation and primary emission contributed substantially to the haze. The mode size of the haze particles was about 0.7 mu m, and the mode size of the post-haze particles was 0.4 mu m, indicating the remarkable growth of particles in haze. However, the ratios of the core size to shell size of core-shell structure soot particles in the haze were similar to those in the post-haze air, suggesting a quick aging of soot particles in either the haze air or the post-haze air. (C) 2016 Elsevier B.V. All rights reserved.

Understanding the evolution of aerosols in the atmosphere is of great importance for improving air quality and reducing aerosol-related uncertainties in global climate simulations. Here, a unique haze episode at a regional receptor site near the East China Sea was examined as a case study of the aging process of atmospheric aerosols during transport. An increase in photochemical age from 5 h. to more than 25 h and a progressive increase in the fitted mean particle diameter from 70 nm to approximately 300 nm were observed. According to the pollution features and meteorology conditions involved, pollution accumulation (PA), sea breeze (SB), and land breeze (LB) periods were identified. Concentrations of black carbon (BC), hydrocarbon-like organic aerosols (HOA), semi-volatile oxidized organic aerosols (SV-OOA), and nitrate increased by 7-fold up to 39-fold when the air masses passed through Taizhou, a nearby city. In addition, nitrate and SV-OOA dominated the aerosol composition in the urban outflow plumes (52% and 18%, respectively), yet they gradually decreased in concentration during transport. In contrast, sulfate and the low-volatile oxidized organic aerosols (LV-OOA) exhibited more regional footprints and potentially have similar formation mechanisms. The atomic oxygen-to-carbon (O/C) ratio also increased from 0.45 to 0.9, thereby suggesting that rapid formation of highly oxidized secondary organic aerosols (SOA) occurred during transport. Overall, these results provide valuable insight into the evolution of the chemical and physical features of aerosol pollution during transport and also highlight the need for regulatory controls of nitrogen oxides, sulfur dioxide, and VOCs to improve air quality on different scales. (C) 2016 Published by Elsevier Ltd.

Black carbon (BC) exerts profound impacts on air quality and climate because of its high absorption cross-section over a broad range of electromagnetic spectra, but the current results on absorption enhancement of BC particles during atmospheric aging remain conflicting. Here, we quantified the aging and variation in the optical properties of BC particles under ambient conditions in Beijing, China, and Houston, United States, using a novel environmental chamber approach. BC aging exhibits two distinct stages, i.e., initial transformation from a fractal to spherical morphology with little absorption variation and subsequent growth of fully compact particles with a large absorption enhancement. The timescales to achieve complete morphology modification and an absorption amplification factor of 2.4 for BC particles are estimated to be 2.3 h and 4.6 h, respectively, in Beijing, compared with 9 h and 18 h, respectively, in Houston. Our findings indicate that BC under polluted urban environments could play an essential role in pollution development and contribute importantly to large positive radiative forcing. The variation in direct radiative forcing is dependent on the rate and timescale of BC aging, with a clear distinction between urban cities in developed and developing countries, i.e., a higher climatic impact inmore polluted environments. We suggest that mediation in BC emissions achieves a cobenefit in simultaneously controlling air pollution and protecting climate, especially for developing countries.