Shui-Ping Wu

Inter-comparison of Seasonal Variation, Chemical Characteristics, and Source Identification of Atmospheric Fine Particles on Both Sides of the Taiwan Strait

The spatiotemporal distribution and chemical composition of atmospheric fine particles in areas around the Taiwan Strait were firstly investigated. Fine particles (PM2.5) were simultaneously collected at two sites on the west-side, one site at an offshore island, and three sites on the east-side of the Taiwan Strait in 2013–2014. Field sampling results indicated that the average PM2.5 concentrations at the west-side sampling sites were generally higher than those at the east-side sampling sites. In terms of chemical composition, the most abundant water-soluble ionic species of PM2.5 were SO42−, NO3−, and NH4+, while natural crustal elements dominated the metallic content of PM2.5, and the most abundant anthropogenic metals of PM2.5 were Pb, Ni and Zn. Moreover, high OC/EC ratios of PM2.5 were commonly observed at the west-side sampling sites, which are located at the downwind of major stationary sources. Results from CMB receptor modeling showed that the major sources of PM2.5 were anthropogenic sources and secondary aerosols at the both sides, and natural sources dominated PM2.5 at the offshore site. A consistent decrease of secondary sulfate and nitrate contribution to PM2.5 suggested the transportation of aged particles from the west-side to the east-side of the Taiwan Strait.

Diurnal variation of nitrated polycyclic aromatic hydrocarbons in PM10 at a roadside site in Xiamen, China

Intensive daytime and nighttime sampling was carried out from 23 Oct to 31 Dec 2008 to investigate the occurrence of nitrated polycyclic aromatic hydrocarbons (NPAHs) in PM10 at a roadside site in Xiamen, China. At the same time, six PM10 samples were collected from a nearby roadway tunnel for comparison. Six NPAHs, namely 9-nitroanthracene, 2- and 3-nitrofluoranthene, 1-nitropyrene, 7-nitrobenz[a]anthracene, and 6-nitrobenzo[a]pyrene, were identified and quantified using GC/MS in negative ion chemical ionization mode. The average total concentration of six NPAHs (sigmaNPAHs) in the cold season (26 Nov-31 Dec) was 2.3 (daytime) and 9.9 (nighttime) times higher than those in the warm season. Significant statistical difference (p < 0.01, 2-tailed) of sigmaNPAHs between daytime and nighttime was found during both the warm and cold seasons. NPAHs were significantly positively correlated with their parent PAHs and nitrogen dioxide but negatively correlated with ambient temperature. The ratio of 2 + 3-nitrofluoranthene to 1-nitropyrene exhibited a similar diurnal pattern as sigmaNPAHs and was generally greater than 5, indicating the importance of secondary atmospheric formation. The diurnal variations of NPAHs were all influenced by the diurnal variations of PAHs, nitrogen dioxide, sunlight, and temperature. The daily inhalable exposure to the six NPAHs in the tunnel was much higher than the roadside values in the warm season but only slightly higher than those in the cold season.

Hexachlorocyclohexane and Dichlorodiphenyltrichloroethane Residues in the Dustfall of Tianjin, China

Heating and nonheating season dustfall samples were collected from 23 sites in Tianjin, China during 2002–2003 to determine residues of hexachlorocyclohexane isomers (α -HCH, β -HCH, γ -HCH, and δ -HCH) and dichlorodiphenyltrichloroethane and metabolites (p,p′-DDE, p,p′-DDD, and p,p′-DDT). Concentrations of Σ HCH (sum of α -, β -, γ -, and δ -HCH) and Σ DDT (sum of p,p′-DDE, p,p′-DDD, and p,p′-DDT) varied in ranges of 10.9–3.16 × 103 and 37.9–1.53 × 103 ng g− 1 dry weight in heating season and in ranges of 6.9–1.12 × 103 and 18.6–626 ng g− 1 dry weight in nonheating season, respectively. It was found that HCHs and DDTs concentrations of the most heating season samples were higher than those of nonheating season samples collected from the same sites. Among studied compounds of the HCH family, β -HCH prevailed in most samples, suggesting a possible volatilization or resuspension from contaminated topsoil. As for DDTs, p,p′-DDT and p,p′-DDE prevailed in most samples, indicating a possible “fresh” input. Correlations between HCHs/DDTs and total organic carbon and particle size are discussed. Atmospheric deposition fluxes were calculated for the heating and nonheating seasons, and the results showed that the annual input of particulate Σ HCH and Σ DDT from air to surface in the studied area of 1.19 × 104 km2 were 89 t and 80 t, respectively.

Properties and cellular effects of particulate matter from direct emissions and ambient sources

ABSTRACT The pollution of particulate matter (PM) is of great concern in China and many other developing countries. It is generally recognized that the toxicity of PM is source and property dependent. However, the relationship between PM properties and toxicity is still not well understood. In this study, PM samples from direct emissions of wood, straw, coal, diesel combustion, cigarette smoking and ambient air were collected and characterized for their physicochemical properties. Their expression of intracellular reactive oxygen species (ROS) and levels of inflammatory cytokines (i.e., tumor necrosis factor-α (TNF-α)) was measured using a RAW264.7 cell model. Our results demonstrated that the properties of the samples from different origins exhibited remarkable differences. Significant increases in ROS were observed when the cells were exposed to PMs from biomass origins, including wood, straw and cigarettes, while increases in TNF-α were found for all the samples, particularly those from ambient air. The most important factor associated with ROS generation was the presence of water-soluble organic carbon, which was extremely abundant in the samples that directly resulted from biomass combustion. Metals, endotoxins and PM size were the most important properties associated with increases in TNF-α expression levels. The association of the origins of PM particles and physicochemical properties with cytotoxic properties is illustrated using a cluster analysis.

Seasonal variation for the ratio of BaP to BeP at different sites in Great Xiamen Bay

From March 2008 to February 2009, PM(10) samples were collected and analyzed for polycyclic aromatic hydrocarbons (PAHs) at eight sampling sites in Great Xiamen Bay, China. Analyses of the seasonal and spatial variations of these compounds revealed the following results. Significantly high levels of PAHs were found in the winter compared to the summer, sometimes exceeding 100 ng m(-3), and the spatial variations were influenced most by the sampling site surroundings. Composition profiles of PAHs of an urban and a rural site were shown to be very similar with a positive correlation coefficient larger than 0.9 at the 0.01 level of significance for the same season. Diagnostic ratios, together with principal component and multiple linear regression analysis, showed that more PAHs were from grass/wood/coal combustion in winter than in other seasons. The ratios of benzo[a]pyrene to benzo[e]pyrene (BaP-BeP) in winter and fall were 0.6-1.7 times higher than those in spring and summer, suggesting the importance of local emissions of PAHs. The BaP-BeP ratios in Kinmen were generally lower than those in Xiamen, indicating that the aging degree of PAHs was higher in Kinmen than in Xiamen. The external input of PAHs from upwind urban and industrial areas was one of the key factors causing high levels of PAHs in PM(10) in Great Xiamen Bay in winter.

Dry deposition of polycyclic aromatic hydrocarbons and its influence on surface soil contamination in Tianjin, China

ISCLT3 dispersion model was applied to calculate the flux of dry deposition of polycyclic aromatic hydrocarbons (PAHs) in Tianjin, China based on a high resolution emission inventory. Field observations of dry deposition at 22 sampling sites were used for model validation. The mean deposition flux densities (and standard deviation) of 15 PAHs were 4.62 +/- 2.99 microg m(-2) d(-1) and 2.75 +/- 1.78 microg m(-2) d(-1) in the heating and the non-heating seasons, respectively, with a time-weighted annual mean of 3.37 +/- 1.81 microg m(-2) d(-1) (based on the durations of the heating and non-heating seasons). High fluxes occurred in the urbanized areas as well as near two coke and gasification facilities. It was revealed that PAH concentrations in surface soil were correlated significantly with both dry deposition and soil organic matter content. Accordingly, a linear regression model was developed for predicting surface soil PAH concentration based on deposition flux density and soil organic matter content.

Biomass burning contributions to urban PM 2.5 along the coastal lines of southeastern China

Levoglucosan (LG), water soluble organic carbon (WSOC) and potassium (K+), and the light absorption at 365 nm (Abs365) of the extracted WSOC are measured in PM2.5 samples collected from November 2011 to July 2013 at four coastal urban sites in southeast China (Fuzhou, Putian, Quanzhou and Xiamen). These species are markers of biomass burning and used to determine the contributions of biomass burning to the PM2.5 burden in these locations. LG and WSOC concentrations exhibited a clear seasonal pattern, with a large enhancement in winter and spring and a minimum in summer, and annual means across all sites of 59.2±46.8 ng m−3 and 2.69±1.21 µg C m−3, respectively. The distinctive seasonal patterns of LG and WSOC are more explained by the East Asian monsoon than the upwind varying emission sources according to the HYSPLIT backward trajectories and MODIS fire spots. Observations produced significant correlation (at the p<0.01 level) between LG and non-sea salt K+ (nss-K+) at each site, but the correlations exhibited no clear seasonal trend. The LG/nss-K+ ratios ranged from 0.03±0.01 to 0.24±0.13 which lay within the limits for the crop residues and/or grass combustion smoke. Stronger correlations were found between WSOC or Abs365 and sulphate than between WSOC and LG. This observation is consistent with the fact that biomass burning is a less important contributor to WSOC and/or brown carbon than is secondary organic aerosol formation and oxidation. The average relative contributions of biomass burning to OC and WSOC in PM2.5 were 8.3 and 15.2 %, respectively, estimated by the measured LG to OC and WSOC (LG/OC and LG/WSOC) ratios in comparison to literature-derived LG/OC and LG/WSOC values for biomass burning smoke. Using the reported conversion factor of LG to PM2.5 for crop straw burning smoke, the LG-estimated PM2.5 contributions from biomass burning exhibited minimum values in summer and higher values in winter and spring. Positive Matrix Factorisation was used to analyse PM2.5 sources, and seven major source factors including biomass burning emissions were resolved. The biomass burning sources contributed 3.75–8.08 % to PM2.5 mass as an annual average while exhibiting a seasonal variability similar to and higher than those of LG-estimated contributions. These results demonstrate that the contribution from biomass burning smoke to PM2.5 – while small – is non-negligible, especially in the winter and spring sampling periods, that is, northeastern monsoon season.

Stack and fugitive emissions of major air pollutants from typical brick kilns in China

Little information exists on emission factors (EFs, quantities of pollutants emitted per unit of fuel consumed) for brick kilns in China, although brick kilns are important emission sources of many air pollutants, and 45% of the worlds bricks are produced in China. In this study, EFs of carbon dioxide (CO2), carbon monoxide (CO), sulfur dioxide (SO2), nitrogen oxides (NOx), particulate matters (PMs), black carbon (BC), organic carbon (OC), and polycyclic aromatic hydrocarbons (PAHs) for brick kilns were derived based on field measurements of a total of 18 brick kilns of major types in China. This was the first study to quantify EFs of both stack and fugitive sources based on a modified carbon balance method that was developed for this study. The EFs of most pollutants, especially the incomplete combustion products in fugitive emissions, were much higher than those for stack emissions, indicating a substantial underestimation of total emissions when leakage is not taken into consideration. This novel method can be applied to quantify emissions from other similar sources with both stack and fugitive emissions.

Chemical characteristics, source apportionment, and regional transport of marine fine particles toward offshore islands near the coastline of northwestern Taiwan Strait

This study aims to investigate the spatiotemporal variation, chemical composition, and source apportionment of marine fine particles (PM2.5) as well as their regional transport toward the Matsu Islands located near the coastline of northwestern Taiwan Strait. Four offshore island sites located at the Matsu Islands were selected to conduct both regular and intensive sampling of marine PM2.5. Water-soluble ionic species, metallic elements, and carbonaceous contents were then analyzed to characterize the chemical characteristics of marine PM2.5. In order to identify the potential sources and their contributions to marine PM2.5, chemical mass balance (CMB) receptor model was employed along with the backward trajectory simulation to resolve the source apportionment of marine PM2.5 and to explore their transport routes in different seasons. The results showed that high PM2.5 concentrations were commonly observed during the northeastern monsoon periods. Additionally, marine PM2.5 concentration decreased from the west to the east with the highest PM2.5 at the Nankang Island and the lowest PM2.5 at the Donyin Island in all seasons, indicating an obvious concentration gradient of PM2.5 transported from the continental areas to the offshore islands. In terms of chemical characteristics of PM2.5, the most abundant water-soluble ions of PM2.5 were secondary inorganic aerosols (SO42−, NO3−, and NH4+) which accounted for 55–81% of water-soluble ions and 29–52% of marine PM2.5. The neutralization ratios of PM2.5 were always less than unity, indicating that NH4+ cannot solely neutralize nss-SO42+ and NO3− in marine PM2.5 at the Matsu Islands. Although crustal elements (Al, Ca, Fe, K, and Mg) dominated the metallic content of marine PM2.5, trace anthropogenic metals (Cd, As, Ni, and Cr) increased significantly during the northeastern monsoon periods, particularly in winter. Organic carbons (OCs) were always higher than elemental carbons (ECs), and the mass ratios of OC and EC were generally higher than 2.2 in all seasons, implying that PM2.5 was likely to be aged particles. During the poor air quality periods, major air mass transport routes were the northern transport and the anti-cyclonic circulation routes. Source apportionment results indicated that fugitive soil dusts and secondary aerosols were the major sources of marine PM2.5 at the Matsu Islands, while, in winter, biomass burning contributed up to 15% of marine PM2.5. This study revealed that cross-boundary transport accounted for 66~84% of PM2.5 at the Matsu Islands, suggesting that marine PM2.5 at the Matsu Islands has been highly influenced by anthropogenic emissions from neighboring Fuzhou City as well as long-range transport from Northeast Asia.