The molecular composition of humic-like 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.

•Molecular and spatial characteristics of particulate organic compounds in coastal atmosphere of East China are reported.•Terrestrial fossil fuels and biomass burning have significant influences on aerosols in coastal atmosphere of East China.•Continental influences are highly dependent on the air mass origins.•Proportion of compounds from photochemical oxidation increased during the long range transport.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 μgC/m3 and 6.9 ± 2.4 μgC/m3, 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/m3, 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.

•Temporal and spatial variation of PM2.5 at a typical coastal city with industrials and dense population was characterized.•Inorganic and organic secondary components were dominant in PM2.5.•Continental air masses had high PM2.5 concentration, while marine air masses had high secondary components proportion.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 μg/m3, 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 Yellow Sea 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.Download high-res image (305KB)Download full-size image

•New particle formation has been frequently observed in diverse environments of China, even in a heavily-polluted atmosphere.•The distinct profiles of particle formation and subsequent growth suggest the nucleation mechanisms should be reconsidered.•This paper systematically summarizes the recent advances, current bottleneck and future directions in studying NPF in China.New particle formation (NPF) studies have been conducted in China since 2004. Formation of new atmospheric aerosol particles has been observed to take place in diverse environments, even under the circumstances of high pre-existing particle loading, challenging the traditional and present understanding of the physicochemical nucleation mechanisms, which have been proposed based on the investigations in clean environments and under laboratory experimental conditions. This paper summarizes the present status and gaps in understanding NPF in China and discusses the main directions opening for future research.

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 in more polluted environments. We suggest that mediation in BC emissions achieves a cobenefit in simultaneously controlling air pollution and protecting climate, especially for developing countries.

As the world’s second largest economy, China has experienced severe haze pollution, with fine particulate matter (PM) recently reaching unprecedentedly high levels across many cities, and an understanding of the PM formation mechanism is critical in the development of efficient mediation policies to minimize its regional to global impacts. We demonstrate a periodic cycle of PM episodes in Beijing that is governed by meteorological conditions and characterized by two distinct aerosol formation processes of nucleation and growth, but with a small contribution from primary emissions and regional transport of particles. Nucleation consistently precedes a polluted period, producing a high number concentration of nano-sized particles under clean conditions. Accumulation of the particle mass concentration exceeding several hundred micrograms per cubic meter is accompanied by a continuous size growth from the nucleation-mode particles over multiple days to yield numerous larger particles, distinctive from the aerosol formation typically observed in other regions worldwide. The particle compositions in Beijing, on the other hand, exhibit a similarity to those commonly measured in many global areas, consistent with the chemical constituents dominated by secondary aerosol formation. Our results highlight that regulatory controls of gaseous emissions for volatile organic compounds and nitrogen oxides from local transportation and sulfur dioxide from regional industrial sources represent the key steps to reduce the urban PM level in China.

Simultaneous measurements of aerosol size, distribution of number, mass, and chemical compositions were conducted in the winter of 2007 in Beijing using a Twin Differential Mobility Particle Sizer and a Micro Orifice Uniform Deposit Impactor. Both material density and effective density of ambient particles were estimated to be 1.61 ± 0.13 g cm–3 and 1.62 ± 0.38 g cm–3 for PM1.8 and 1.73 ± 0.14 g cm–3 and 1.67 ± 0.37 g cm–3 for PM10. Effective density decreased in the nighttime, indicating the primary particles emission from coal burning influenced the density of ambient particles. Size-resolved material density and effective density showed that both values increased with diameter from about 1.5 g cm–3 at the size of 0.1 μm to above 2.0 g cm–3 in the coarse mode. Material density was significantly higher for particles between 0.56 and 1.8 μm during clean episodes. Dynamic Shape Factors varied within the range of 0.95–1.13 and decreased with particle size, indicating that coagulation and atmospheric aging processes may change the shape of particles.

Ambient aerosol samples were collected at an urban site and an upwind rural site of Beijing during the CAREBEIJING-2008 (Campaigns of Air quality REsearch in BEIJING and surrounding region) summer field campaign. Contributions of primary particles and secondary organic aerosols (SOA) were estimated by chemical mass balance (CMB) modeling and tracer-yield method. The apportioned primary and secondary sources explain 73.8% ± 9.7% and 79.6% ± 10.1% of the measured OC at the urban and rural sites, respectively. Secondary organic carbon (SOC) contributes to 32.5 ± 15.9% of the organic carbon (OC) at the urban site, with 17.4 ± 7.6% from toluene, 9.7 ± 5.4% from isoprene, 5.1 ± 2.0% from α-pinene, and 2.3 ± 1.7% from β-caryophyllene. At the rural site, the secondary sources are responsible for 38.4 ± 14.4% of the OC, with the contributions of 17.3 ± 6.9%, 13.9 ± 9.1%, 5.6 ± 1.9%, and 1.7 ± 1.0% from toluene, isoprene, α-pinene, and β-caryophyllene, respectively. Compared with other regions in the world, SOA in Beijing is less aged, but the concentrations are much higher; between the sites, SOA is more aged and affected by regional transport at the urban site. The high SOA loading in Beijing is probably attributed to the high regional SOC background (∼2 μg m–3). The toluene SOC concentration is high and comparable at the two sites, implying that some anthropogenic components, at least toluene SOA, are widespread in Beijing and represents a major factor in affecting the regional air quality. The aerosol gaseous precursor concentrations and temperature correlate well with SOA, both affecting SOA formation. The significant SOA enhancement with increasing water uptake and acidification indicates that the aqueous-phase reactions are largely responsible SOA formation in Beijing.

Little is known about the characteristics of particulate matter emissions from vehicles in China, although such information is critical in source apportionment modeling, emission inventories, and health effect studies. In this paper, we report a comprehensive characterization of PM2.5 emissions in the Zhujiang Tunnel in the Pearl River Delta region of China. The chemical speciation included elemental carbon, organic carbon, inorganic ions, trace elements, and organic compounds. The emission factors of individual species and their relative distributions were obtained for a mixed fleet of heavy-duty vehicles (19.8%) and light-duty vehicles (80.2%). In addition, separate emission factors of PM2.5 mass, elemental carbon, and organic matter for heavy-duty vehicles and light-duty vehicles also were derived. As compared to the results of other tunnel studies previously conducted, we found that the abundances and distributions of the trace elements in PM2.5 emissions were more varied. In contrast, the characteristics of the trace organic compounds in the PM2.5 emissions in our study were consistent with characteristics found in other tunnel studies and dynamometer tests. Our results suggested that vehicular PM2.5 emissions of organic compounds are less influenced by the geographic area and fleet composition and thereby are more suitable for use in aerosol source apportionment modeling implemented across extensive regions.

Dry-deposited particles were collected during the passage of an extremely strong dust storm in March, 2010 at a coastal site in Qingdao (36.15°N, 120.49°E), a city located in Eastern China. The size, morphology, and elemental composition of the particles were quantified with a scanning electron microscope equipped with an energy dispersive X-ray instrument (SEM–EDX). The particles appeared in various shapes, and their size mainly varied from 0.4 to 10 μm, with the mean diameters of 0.5, 1.5, and 1.0 μm before, during, and after the dust storm, respectively. The critical size of the mineral particles settling on the surface in the current case was about 0.3–0.4 μm before the dust storm and about 0.5–0.7 μm during the dust storm. Particles that appeared in high concentration but were smaller than the critical size deposited onto the surface at a small number flux. The elements Al, Si and Mg were frequently detected in all samples, indicating the dominance of mineral particles. The frequency of Al in particles collected before the dust storm was significantly lower than for those collected during and after the dust storm. The frequencies of Cl and Fe did not show obvious changes, while those of S, K and Ca decreased after the dust arrival. These results indicate that the dust particles deposited onto the surface were less influenced by anthropogenic pollutants in terms of particle number.Dry deposited dust particles on China coast were analyzed by SEM. In comparison with the suspended particles, the critical size for dry deposited dust particles was 0.5–0.7 μm.Download full-size image