Lingxiao Yang

Airborne particulate polycyclic aromatic hydrocarbon (PAH) pollution in a background site in the North China Plain: Concentration, size distribution, toxicity and sources

The size-fractionated characteristics of particulate polycyclic aromatic hydrocarbons (PAHs) were studied from January 2011 to October 2011 using a Micro-orifice Uniform Deposit Impactor (MOUDI) at the Yellow River Delta National Nature Reserve (YRDNNR), a background site located in the North China Plain. The average annual concentration of total PAHs in the YRDNNR (18.95 ± 16.51 ng/m(3)) was lower than that in the urban areas of China; however, it was much higher than that in other rural or remote sites in developed countries. The dominant PAHs, which were found in each season, were fluorene (5.93%-26.80%), phenanthrene (8.17%-26.52%), fluoranthene (15.23%-27.12%) and pyrene (9.23%-16.31%). A bimodal distribution was found for 3-ring PAHs with peaks at approximately 1.0-1.8 μm and 3.2-5.6 μm; however, 4-6 ring PAHs followed a nearly unimodal distribution, with the highest peak in the 1.0-1.8 μm range. The mass median diameter (MMD) values for the total PAHs averaged 1.404, 1.467, 1.218 and 0.931 μm in spring, summer, autumn and winter, respectively. The toxicity analysis indicated that the carcinogenic potency of particulate PAHs existed primarily in the <1.8 μm size range. Diagnostic ratios and PCA analysis indicated that the PAHs in aerosol particles were mainly derived from coal combustion. In addition, back-trajectory calculations demonstrated that atmospheric PAHs were produced primarily by local anthropogenic sources.

Sources apportionment of PM2.5 in a background site in the North China Plain

To better understand the sources and potential source regions of PM2.5, a field study was conducted from January 2011 to November 2011 at a background site, the Yellow River Delta National Nature Reserve (YRDNNR) in the North China Plain. Positive matrix factorisation (PMF) analysis and a potential source contribution function (PSCF) model were used to assess the data, which showed that YRDNNR experienced serious air pollution. Concentrations of PM2.5 at YRDNNR were 71.2, 92.7, 97.1 and 62.5 μg m(-3) in spring, summer, autumn and winter, respectively, with 66.0% of the daily samples exhibiting higher concentrations of PM2.5 than the national air quality standard. PM2.5 mass closure showed remarkable seasonal variations. Sulphate, nitrate and ammonium were the dominant fractions of PM2.5 in summer (58.0%), whereas PM2.5 was characterized by a high load of organic aerosols (40.2%) in winter. PMF analysis indicated that secondary sulphate and nitrate (54.3%), biomass burning (15.8%), industry (10.7%), crustal matter (8.3%), vehicles (5.2%) and copper smelting (4.9%) were important sources of PM2.5 at YRDNNR on an annual average. The source of secondary sulphate and nitrate was probably industrial coal combustion. PSCF analysis indicated a significant regional impact on PM2.5 at YRDNNR all year round. Local emission may be non-negligible at YRDNNR in summer. The results of the present study provide a scientific basis for the development of PM2.5 control strategies on a regional scale.

Individual metal-bearing particles in a regional haze caused by firecracker and firework emissions

Intensive firecracker/firework displays during Chinese New Year (CNY) release fine particles and gaseous pollutants into the atmosphere, which may lead to serious air pollution. We monitored ambient PM(2.5) and black carbon (BC) concentrations at a regional background site in the Yellow River Delta region during the CNY in 2011. Our monitoring data and MOUDI images showed that there was a haze event during the CNY. Daily average PM(2.5) concentration reached 183 μg m(-3) during the CNY, which was six times higher than that before and after the CNY. Similarly, the black carbon (BC) concentrations were elevated during the CNY. In order to confirm whether the firecracker/firework related emission is the main source of the haze particles, we further analyzed the morphology and chemical composition of individual airborne particles collected before, during and after the CNY by using transmission electron microscopy coupled with energy-dispersive X-ray spectroscopy (TEM/EDS). We found that sulfate and organic-rich particles were dominant in the atmosphere before and after the CNY. In contrast, K-rich sulfates and other metal (e.g., Ba-rich, Al-rich, Mg-rich, and Fe-rich) particles were much more abundant than ammoniated sulfate particles during the CNY. These data suggest that it was the aerosol particles from the firecracker/firework emissions that induced the regional haze episode during the CNY. In individual organic and K-rich particles, we often found more than two types of nano-metal particles. These metal-bearing particles also contained abundant S but not Cl. In contrast, fresh metal-bearing particles from firecrackers generated in the laboratory contained abundant Cl with minor amounts of S. This indicates that the firecracker/firework emissions during the CNY significantly changed the atmospheric transformation pathway of SO(2) to sulfate.

Mixing state and hygroscopicity of dust and haze particles before leaving Asian continent

Pollutants during haze and Asian dust storms are transported out of the Asian continent, affecting the regional climate and the hydrological and biogeochemical cycles. Understanding the physicochemical properties of aerosol particles is essential to quantify their impacts. In order to determine physicochemical properties of aerosols before leaving the Asian continent, we carried out a field campaign from 14 April to 2 May 2011 at a background site in the path of Asian dust and haze outflows. We measured concentrations of gaseous pollutants (SO2, NO2, NO, O3, and CO), black carbon (BC), and particle number in situ and collected airborne particles for microscopic analysis. Pollutant concentrations (BC, 4 µg m−3; CO, 808 ppb; SO2, 24 ppb; NO2, 37 ppb) were highest during haze periods, except for PM2.5 mass, which was highest (162 µg m−3) during a dust storm. Seventy-one percent of haze particles were coated with organic films and 32% were internal mixtures of sulfates and refractory particles (e.g., soot, metal/fly ash, and mineral). Seventy-nine percent of haze particles have deliquescence relative humidity at 68–70%. During a dust storm, soot particles were observed among dust particles. Most dust particles were hydrophobic, and no Ca(NO3)2 was observed in dust particles collected during the dust storms, but up to 32% of dust particles were found to be coated with Ca(NO3)2 after the main dust storm moved out of the sampling area. These results indicated that both natural and anthropogenic aerosol particles in Asian outflow can undergo significant physicochemical processes before leaving the Asian continent.

Radiative absorption enhancement from coatings on black carbon aerosols.

The radiative absorption enhancement of ambient black carbon (BC), by light-refractive coatings of atmospheric aerosols, constitutes a large uncertainty in estimates of climate forcing. The direct measurements of radiative absorption enhancement require the experimentally-removing the coating materials in ambient BC-containing aerosols, which remains a challenge. Here, the absorption enhancement of the BC core by non-absorbing aerosol coatings was quantified using a two-step removal of both inorganic and organic matter coatings of ambient aerosols. The mass absorption cross-section (MAC) of decoated/pure atmospheric BC aerosols of 4.4±0.8m(2)g(-1) was enhanced to 9.6±1.8m(2)g(-1) at 678-nm wavelength for ambiently-coated BC aerosols at a rural Northern China site. The enhancement of MAC (EMAC) rises from 1.4±0.3 in fresh combustion emissions to ~3 for aged ambient China aerosols. The three-week high-intensity campaign observed an average EMAC of 2.25±0.55, and sulfates were primary drivers of the enhanced BC absorption.

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.

Characteristics of carbonaceous aerosols: Impact of biomass burning and secondary formation in summertime in a rural area of the North China Plain

To determine the characteristics of carbonaceous aerosols in rural areas of the North China Plain, field measurements were conducted at Yucheng (YC) in the summers of 2013 and 2014. The concentrations of carbonaceous aerosols at YC exhibited clear diurnal variation, with higher concentrations in the early morning and at night and lower concentrations during the afternoon hours. The mass-balance method designed for particulate matter smaller than 2.5μm (PM2.5) was used to calculate the organic matter (OM)/organic carbon (OC) ratio. The value obtained, 2.07±0.05, was suggested as a reference to estimate organics in PM2.5 in rural areas of the North China Plain. Biomass burning was identified to be a significant source of carbonaceous aerosols; approximately half of the samples obtained at YC were affected by biomass burning during summer 2013. Case studies revealed that biomass burning accounted for up to 52.6% of the OC and 51.1% of the elemental carbon in PM2.5 samples. The organic coatings observed on sulphur-rich and potassium-rich particles indicated the formation of secondary organic aerosols (SOA) from the oxidation of precursor volatile organic compounds (VOCs) during the aging of smoke released from biomass burning. Based on the evolution of the VOCs, the contribution of VOCs oxidation to SOA concentration was 3.21 and 1.07μgm(-3)ppm(-1) CO under conditions of low nitrogen oxide (NOx) and high NOx, respectively. Aromatics (e.g. benzene, toluene, xylene and ethylbenzene) made the greatest contribution to SOA concentration (88.4% in low-NOx conditions and 80.6% in high-NOx conditions). The results of the study offer novel insights into the effects of biomass burning on the carbonaceous aerosols and SOA formation in polluted rural areas.

Levels, indoor-outdoor relationships and exposure risks of airborne particle-associated perchlorate and chlorate in two urban areas in Eastern Asia.

Indoor and outdoor concentrations of PM2.5-associated perchlorate (ClO4(-)) and chlorate (ClO3(-)) were investigated in Jinan, China, and size-resolved perchlorate and chlorate were studied in Kumamoto, Japan. The average outdoor PM2.5-associated concentrations of perchlorate and chlorate were 4.18 ng m(-3) and 2.82 ng m(-3), respectively, in Jinan. Perchlorate and chlorate were mainly distributed in fine particles, and their approximate PM2.5-associated concentrations were 0.04 ng m(-3) and 4.14 ng m(-3), respectively, in Kumamoto. The ratios of ClO3(-)/ClO4(-) ranged from 18.72 to 360.22 in Kumamoto and from 0.03 to 7.45 in Jinan. The highest concentration of perchlorate (173.76 ng m(-3)) was observed on Spring Festival Eve. This finding and the significant correlation between perchlorate and fireworks-related components (Cl(-) and K(+)) indicated that the fireworks display was a significant source of perchlorate in Jinan. The indoor concentrations of perchlorate and chlorate in Jinan were 3.54 ng m(-3) (range, 0.14-125.14 ng m(-3)) and 0.94 ng m(-3) (range, 0.10-1.80 ng m(-3)), respectively. In the absence of an indoor source of perchlorate, the occurrence of indoor concentrations higher than those found outdoors was a common effect of individual fireworks displays near the sampling sites, coupled with meteorological influences and poor indoor diffusion conditions. The exposure risks of perchlorate and chlorate indoors indicated that the potential risk of perchlorate exposure to children during fireworks displays is deserving of concern.

Particle size distributions, PM 2.5 concentrations and water-soluble inorganic ions in different public indoor environments: a case study in Jinan, China

In this study, we collected particles with aerodynamic diameter ⩽2.5 μm (PM2.5) from three different public indoor places (a supermarket, a commercial office, and a university dining hall) in Jinan, a medium-sized city located in northern China. Water-soluble inorganic ions of PM2.5 and particle size distributions were also measured. Both indoor and outdoor PM2.5 levels (102.3–143.8 μg·m−3 and 160.2–301.3 μg·m−3, respectively) were substantially higher than the value recommended by the World Health Organization (25 μg·m−3), and outdoor sources were found to be the major contributors to indoor pollutants. Diurnal particle number size distributions were different, while the maximum volume concentrations all appeared to be approximately 300 nm in the three indoor locations. Concentrations of indoor and outdoor PM2.5 were shown to exhibit the same variation trends for the supermarket and dining hall. For the office, PM2.5 concentrations during nighttime were observed to decrease sharply. Among others, SO42−, NH4+ and NO3− were found to be the dominant water-soluble ions of both indoor and outdoor particles. Concentrations of NO3− in the supermarket and office during the daytime were observed to decrease sharply, which might be attributed to the fact that the indoor temperature was much higher than the outdoor temperature. In addition, domestic activities such as cleaning, water usage, cooking, and smoking also played roles in degraded indoor air quality. However, the results obtained here might be negatively impacted by the small number of samples and short sampling durations.