Xiaomei Gao

Polluted dust promotes new particle formation and growth

Understanding new particle formation and their subsequent growth in the troposphere has a critical impact on our ability to predict atmospheric composition and global climate change. High pre-existing particle loadings have been thought to suppress the formation of new atmospheric aerosol particles due to high condensation and coagulation sinks. Here, based on field measurements at a mountain site in South China, we report, for the first time, in situ observational evidence on new particle formation and growth in remote ambient atmosphere during heavy dust episodes mixed with anthropogenic pollution. Both the formation and growth rates of particles in the diameter range 15–50 nm were enhanced during the dust episodes, indicating the influence of photo-induced, dust surface-mediated reactions and resulting condensable vapor production. This study provides unique in situ observations of heterogeneous photochemical processes inducing new particle formation and growth in the real atmosphere, and suggests an unexpected impact of mineral dust on climate and atmospheric chemistry.

Impacts of firecracker burning on aerosol chemical characteristics and human health risk levels during the Chinese New Year Celebration in Jinan, China

Measurements for size distribution and chemical components (including water-soluble ions, OC/EC and trace elements) of particles were taken in Jinan, China, during the 2008 Chinese New Year (CNY) to assess the impacts of firecracker burning on aerosol chemical characteristics and human health risk levels. On the eve of the CNY, the widespread burning of firecrackers had a clear contribution to the number concentration of small accumulation mode particles (100-500 nm) and PM2.5 mass concentration, with a maximum PM2.5 concentration of 464.02 μg/m(3). The firecracker activities altered the number size distribution of particles, but had no influence on the mass size distribution of major water-soluble ions. The concentrations of aerosol and most ions peaked in the rush hour of firecracker burning, whereas the peaks of NO3(-) and NH4(+) presented on the day following the burning of firecrackers. K(+), SO4(2-) and Cl(-) composed approximately 62% of the PM2.5 mass, and they existed as KCl and K2SO4 during the firecracker period. However, during the non-firecracker period, organic matter (OM), SO4(2-), NO3(-) and NH4(+) were the major chemical components of the PM2.5, and major ions were primarily observed as (NH4)2SO4 and NH4NO3. Estimates of non-carcinogenic risk levels to human health showed that the elemental risk levels during the firecracker period were substantially higher than those observed during the non-firecracker period. The total elemental risk levels in Jinan for the three groups (aged 2-6 years, 6-12 years and ≥70 years) were higher than 2 during the firecracker period, indicating that increased pollutant levels emitted from the burning of firecrackers over short periods of time may cause non-carcinogenic human health risks.

Evaluating PM2.5 ionic components and source apportionment in Jinan, China from 2004 to 2008 using trajectory statistical methods

The mass concentrations and major chemical components of PM(2.5) in Jinan, Shandong Province, China from Dec. 2004 to Oct. 2008 were analyzed using backward trajectory cluster analysis in conjunction with the potential source contribution function (PSCF) model. The aim of this work was to study the inter-annual variations of mass concentrations and major chemical components of PM(2.5), evaluate the air mass flow patterns and identify the potential local and regional source areas that contributed to secondary sulfate and nitrate in PM(2.5) in Jinan. The annual mean concentrations of PM(2.5), sulfate and nitrate in 2004-2008 were almost the highest in the world. The most significant air parcels contributing to the highest mean concentrations of mass and secondary ions in PM(2.5) originated from the industrialized areas of Shandong Province. Clusters with a lower ratio of NO(3)(-)/SO(4)(2-) in PM(2.5) originated from the Yellow Sea, while a higher ratio was observed in the clusters passing through Beijing and Tianjin. PSCF modeling indicated that the provinces of Shandong, Henan, Jiangsu, Anhui and the Yellow Sea were the major potential source regions for sulfate, in agreement with the cluster analysis results. Regional and long-range transport of NH(4)NO(3) played an important role in the nitrate concentration of Jinan. By comparing the distributions of secondary sulfate and nitrate over three years, enhanced emission control management before and during the 29(th) Olympic Games led to a discernible decrease in source contributions from Beijing and its environs in 2007-2008.

Aerosol ionic components at Mt. Heng in central southern China: Abundances, size distribution, and impacts of long-range transport

Water-soluble ions in PM(2.5) were continuously measured, along with the measurements of many other species and collection of size-resolved aerosol samples, at the summit of Mt. Heng in the spring of 2009, to understand the sources of aerosols in rural central southern China. The mean concentrations of SO(4)(2-), NH(4)(+) and NO(3)(-) in PM(2.5) were 8.02, 2.94 and 1.47 μg/m(3), indicating a moderate aerosol pollution level at Mt. Heng. Water-soluble ions composed approximately 40% of the PM(2.5) mass on average. PM(2.5) was weakly acidic with about 66% of the samples being acidic. SO(4)(2-), NO(3)(-) and NH(4)(+) exhibited similar diurnal patterns with a broad afternoon maximum. SO(4)(2-) and NH(4)(+) were mainly present in the fine aerosols with a peak in the droplet mode of 0.56-1 μm, suggesting the important role of cloud processing in the formation of aerosol sulfate. NO(3)(-) was largely distributed in the coarse particles with a predominant peak in the size-bin of 3.2-5.6 μm. Long-distance transport of processed air masses, dust aerosols, and cloud/fog processes were the major factors determining the variations of fine aerosol at Mt. Heng. The results at Mt. Heng were compared with those obtained from our previous study at Mt. Tai in north China. The comparison revealed large differences in the aerosol characteristics and processes between southern and northern China. Backward trajectories indicated extensive transport of anthropogenic pollution from the coastal regions of eastern/northern China and the Pearl River Delta (PRD) to Mt. Heng in spring, highlighting the need for regionally coordinated control measures for the secondary pollutants.

On the use of an explicit chemical mechanism to dissect peroxy acetyl nitrate formation

Peroxy acetyl nitrate (PAN) is a key component of photochemical smog and plays an important role in atmospheric chemistry. Though it has been known that PAN is produced via reactions of nitrogen oxides (NOx) with some volatile organic compounds (VOCs), it is difficult to quantify the contributions of individual precursor species. Here we use an explicit photochemical model--Master Chemical Mechanism (MCM) model--to dissect PAN formation and identify principal precursors, by analyzing measurements made in Beijing in summer 2008. PAN production was sensitive to both NOx and VOCs. Isoprene was the predominant VOC precursor at suburb with biogenic impact, whilst anthropogenic hydrocarbons dominated at downtown. PAN production was attributable to a relatively small class of compounds including NOx, xylenes, trimethylbenzenes, trans/cis-2-butenes, toluene, and propene. MCM can advance understanding of PAN photochemistry to a species level, and provide more relevant recommendations for mitigating photochemical pollution in large cities.

Size distributions of aerosol sulfates and nitrates in Beijing during the 2008 Olympic Games: Impacts of pollution control measures and regional transport

For the 2008 Olympic Games, drastic control measures were implemented on industrial and urban emissions of sulfur dioxide (SO2), nitrogen oxides (NOx) and other pollutants to address the issues of poor air quality in Beijing. To investigate the effects of SO2 and NOx reductions on the particulate sulfate and nitrate concentrations as well as their size distributions, size-segregated aerosol samples were collected using micro-orifice uniform deposit impactors (MOUDIs) at urban and downwind rural sites in Beijing before and after full-scale controls. During the sampling period, the mass concentrations of fine particles (PM1.8) at the urban and rural sites were 94.0 and 85.9 μg m−3, respectively. More than 90% of the sulfates and ∼60% of nitrates formed as fine particles. Benefiting from the advantageous meteorological conditions and the source controls, sulfates were observed in rather low concentrations and primarily in condensation mode during the Olympics. The effects of the control measures were separately analyzed for the northerly and the southerly air-mass-dominated days to account for any bias. After the control measures were implemented, PM, sulfates, and nitrates were significantly reduced when the northerly air masses prevailed, with a higher percentage of reduction in larger particles. The droplet mode particles, which dominated the sulfates and nitrates before the controls were implemented, were remarkably reduced in mass concentration after the control measures were implemented. Nevertheless, when the polluted southerly air masses prevailed, the local source control measures in Beijing did not effectively reduce the ambient sulfate concentration due to the enormous regional contribution from the North China Plain.

Size-resolved aerosol ionic composition and secondary formation at Mount Heng in South Central China

To understand the size-resolved aerosol ionic composition and the factors influencing secondary aerosol formation in the upper boundary layer in South Central China, size-segregated aerosol samples were collected using a micro-orifice uniform deposit impactor (MOUDI) in spring 2009 at the summit of Mount Heng (1269 m asl), followed by subsequent laboratory analyses of 13 inorganic and organic water-soluble ions. During non-dust-storm periods, the average PM1.8 concentration was 41.8 μg·m-3, contributing to 55% of the PM10. Sulfates, nitrates, and ammonium, the dominant ions in the fine particles, amounted to 46.8% of the PM1.8. Compared with Mount Tai in the North China Plain, the concentrations of both fine and coarse particles and the ions contained therein were substantially lower. When the air masses from Southeast Asia prevailed, intensive biomass burning there led to elevated concentrations of sulfates, nitrates, ammonium, potassium, and chloride in the fine particles at Mount Heng. The air masses originating from the north Gobi brought heavy dust storms that resulted in the remarkable production of sulfates, ammonium, methane sulfonic acid, and oxalates in the coarse particles. Generally, the sulfates were primarily produced in the form of (NH4)2SO4 in the droplet mode via heterogeneous aqueous reactions. Only approximately one-third of the nitrates were distributed in the fine mode, and high humidity facilitated the secondary formation of fine nitrates. The heterogeneous formation of coarse nitrates and ammonium on dry alkaline dust surfaces was found to be less efficient than that on the coarse particles during non-dust-storm periods.