Meng-Der Fang

Distribution and source recognition of polycyclic aromatic hydrocarbons in the sediments of Hsin-ta Harbour and adjacent coastal areas, Taiwan

Thirty-three sediment samples from Hsin-ta Harbour and neighboring coastal areas were analyzed by GC-MS for polycyclic aromatic hydrocarbons (PAHs). Total concentrations of 30 analyzed parental and alkylated PAHs ( summation operator PAH) varied from 98.1 to 3382 ng/g dry weight. MP/P (methylphenanthrenes/phenanthrene) values larger than 2 coincided with very low P/A (phenanthrene/anthracene) values at inner harbour stations, revealing that a significant portion of low molecular weight PAHs are probably from petrogenic pollution sources, specifically, illegal disposal of used motor oil. The 4,6-dimethyldibenzothiophene/3,6-dimethylphenanthrene (4,6-C(2)D/3,6-C(2)P) ratio is found to be more useful than the MP/P ratio in tracing petrogenic PAHs from the inner harbour area to the adjacent coastal environment. In addition, according to hierarchical cluster analysis, collected sediments cluster in three major groups, Off-shore Group, Near-shore Group and Inner Harbour Group. Three diagnostic ratios, 4,6-C(2)D/3,6-C(2)P, PER/ summation operator PAH (perylene to summation operator PAH) and BaA/CHR (benzo(a)anthracene/chrysene), representing petrogenic, biogenic and pyrogenic origins, are found to be effective in differentiating and characterizing sediments among the groups in this study. Enrichment of pyrogenic and petrogenic PAHs in sediments collected exhibits mixing or dilution, spatially, by biogenic (or natural) PAHs.

Polycyclic aromatic hydrocarbons in coastal sediments of southwest Taiwan: An appraisal of diagnostic ratios in source recognition

Fifty-seven surface sediment samples were collected from the coast of southwest Taiwan and analyzed for polycyclic aromatic hydrocarbons (PAHs). Concentrations of total PAHs (28 PAH compounds) ranged from 15 to 907 ng g(-1) dry weight. Diagnostic ratios showed that PAHs in the sediments of the Gaoping estuary were predominantly of petroleum origin, whereas sediments from the Kaohsiung coast contained principally combustion-derived PAHs. Principal component analysis indicated that emissions from automobiles and coal burning were the main sources of combustion-derived PAHs. The relatively high ratios of perylene/penta-aromatic PAH isomers in sediments from the Tainan coast and some off-shore stations on the Kaohsiung coast suggest a significant diagenetic PAH contribution. The study shows that certain diagnostic ratios are useful and sensitive in delineating the distribution of PAHs from specific sources in southwest Taiwan. The phenanthrene/anthracene ratio is a better indicator than the methylphenanthrenes/phenanthrene ratio for tracing petrogenic PAHs, and the benzo(a)anthracene/chrysene and indeno(1,2,3-c,d)pyrene/benzo(g,h,i)perylene ratios are more specific than the benzo(a)pyrene/benzo(e)pyrene and benzo(b)fluoranthcene/benzo(k)fluoranthcene ratios in distinguishing PAHs from various pyrogenic sources.

Emerging organic contaminants in coastal waters: Anthropogenic impact, environmental release and ecological risk

This study provides a first estimate of the sources, distribution, and risk presented by emerging organic contaminants (EOCs) in coastal waters off southwestern Taiwan. Ten illicit drugs, seven nonsteroidal anti-inflammatory drugs (NSAIDs), five antibiotics, two blood lipid regulators, two antiepileptic drugs, two UV filters, caffeine, atenolol, and omeprazole were analyzed by solid-phase extraction and liquid chromatography coupled to tandem mass spectrometry (SPE-LC-MS/MS). Thirteen EOCs were detected in coastal waters, including four NSAIDs (acetaminophen, ibuprofen, ketoprofen, and codeine), three antibiotics (ampicillin, erythromycin, and cefalexin), three illicit drugs (ketamine, pseudoephedrine, and MDMA), caffeine, carbamazepine, and gemfibrozil. The median concentrations for the 13 EOCs ranged from 1.47 ng/L to 156 ng/L. Spatial variation in concentration of the 13 EOCs suggests discharge into coastal waters via ocean outfall pipes and rivers. Codeine and ampicillin have significant pollution risk quotients (RQ>1), indicating potentially high risk to aquatic organisms in coastal waters.

Polybrominated diphenyl ethers and polychlorinated biphenyls in sediments of southwest Taiwan: Regional characteristics and potential sources

Very little information is available on the contamination of coastal sediments of Taiwan by PBDEs and PCBs. In this study, we determined the concentrations of 19 PBDE and 209 PCB congeners in 57 surface sediment samples to identify the possible sources of PBDEs and PCBs. The total PBDE and PCB concentrations ranged from below detection limit to 7.73 ng/g and 0.88-7.13 ng/g, respectively; these values are within the ranges observed for most coastal sediments worldwide. The PBDE congeners were dominated by BDE-209 (50.7-99.7%), with minor contributions from penta- and octa-BDEs. The signatures of PCB congeners suggested that PCB residues in Kaohsiung coast may be the legacy of past use or the result of ongoing inputs from the maintenance, repair and salvage of old ships. Principal component analysis of the congener-specific composition of PBDEs and PCBs revealed distinct regional patterns that are related to the use of commercial products.

Concentrations of chlorobenzenes, hexachlorobutadiene and heavy metals in surficial sediments of Kaohsiung coast, Taiwan

This work analyzes surface sediment samples collected from 40 stations along the Kaohsiung coast in southern Taiwan for chlorobenzenes (CBs), hexachlorobutadiene (HCBD) and heavy metals (Cu, Zn, Pb, Cd, Ni, Fe, Mn and Cr). The highest CBs concentrations are recorded in station T7-15 (about 10 km west off the outlet of Da-lin-pu ocean outfall pipe), with total di-, tri-, tetra-, penta- and hexa-chlorobenzenes concentrations of 290.5, 117.1, 64.5, 15.7 and 22.3 ng/g, respectively. The major pollution source of HCBD is most likely located in the Tso-yin ocean outfall field; while the Dah-lin-pu ocean outfall field and Kao-ping Chi estuary, located in the southern portion of Kaohsiung coast, are the major contributors of hexachlorobenzene. The concentration of CBs congeners correlate fairly well with each other, as do metals. However, concentrations of organics (CBs and HCBD) did not correlate with metals. This finding implies that the pollution characteristics of organics and heavy metals in this highly utilized coastal zone markedly differ from each other.

Sources and distribution of chlorobenzenes and hexachlorobutadiene in surficial sediments along the coast of Southwestern Taiwan

Abstract The spatial distribution of chlorobenzenes in surficial sediments of the estuaries of major rivers along the coast of southwestern Taiwan was determined. Analytical results from sediment sampling stations indicate that the three outfall fields near Taiwans largest industrial city, Kaohsiung, exhibit the highest concentrations of chlorobenzenes. More specifically, sediments from Tso-yin outfall field, which receives the wastewater from a very large petrochemical complex, had concentrations of 1,3,5-trichlorobenzene, pentachlorobenzene, hexachlorobenzene and hexachlorobutadiene 2–3 times higher than those from Chon-chou and Da-lin-pu outfall fields. Chlorobenzene congeners in sediments from the three outfall fields correlate closely and most of their correlation coefficients are even higher than those reported for Ise Bay, Japan. Results from undeveloped areas, estuaries of the Da-du, Tso-shui, and Chi-shui Chi, will be of value after the impact of planned industrial expansion development begins.

Air-water exchange fluxes of polycyclic aromatic hydrocarbons in the tropical coast, Taiwan.

Air-water exchange fluxes of polycyclic aromatic hydrocarbons (PAHs) were simultaneously measured in air and water samples from two sites on the Kenting coast, located at the southern tip of Taiwan, from January to December 2010. There was no significant difference in the total PAH (t-PAH) concentrations in both gas and dissolved phases between these two sites due to the less local input which also coincided to the low levels of t-PAH concentration; the gas and dissolved phases averaged 1.29±0.59 ng m(-3) and 2.17±1.19 ng L(-1) respectively. The direction and magnitude of the daily flux of PAHs were significantly influenced by wind speed and dissolved PAH concentrations. Individual PAH flux ranged from 627 ng m(-2) d(-1) volatilization of phenanthrene during the rainy season with storm-water discharges raising dissolved phase concentration, to 67 ng m(-2) d(-1) absorption of fluoranthene during high wind speed periods. Due to PAH annual fluxes through air-water exchange, Kenting seawater is a source of low molecular weight PAHs and a reservoir of high molecular weight PAHs. Estimated annual volatilization fluxes ranged from 7.3 μg m(-2) yr(-1) for pyrene to 50 μg m(-2) yr(-1) for phenanthrene and the absorption fluxes ranged from -2.6 μg m(-2) yr(-1) for chrysene to -3.5 μg m(-2) yr(-1) for fluoranthene.

Diffusive exchange of PAHs across the air–water interface of the Kaohsiung Harbor lagoon, Taiwan

Instantaneous air-water polycyclic aromatic hydrocarbons (PAHs) exchange fluxes were calculated in 22 pairs of ambient air and water samples from Kaohsiung Harbor lagoon, from December 2003 to January 2005. The highest net volatilization (3135 ng m(-2) day(-1)) and absorptive (-1150 ng m(-2) day(-1)) fluxes in the present study were obtained for the three-ring PAH phenanthrene on 7 April and 27 January 2004, respectively. All PAH diffusive fluxes for three-ring PAHs except phenanthrene were mainly volatilization exchange across the air-water interface. Phenanthrene and the four-ring PAHs were absorbed primarily from the atmosphere and deposited to the surface water, although some minor volatilization fluxes were also observed. Differences in flux magnitude and direction between the dry and wet seasons were also evident for PAHs. Strong absorptive/weaker volatilization PAH fluxes occurred in the dry season, but the opposite was found in the wet season. The mean daily PAH diffusive fluxes were an in flux of -635 ng m(-2) day(-1) in the dry season and an efflux of 686 ng m(-2) day(-1) in the wet season. The integrated absorbed and emitted fluxes of PAHs for harbor lagoon surface waters in the dry and wet seasons were 3.1 kg and 3.4 kg, respectively. Different from water bodies located in temperate zone, phenanthrene diffusive fluxes in Kaohsiung Harbor lagoon was favored in volatilization from surface waters during the wet season (April to September) because of scavenging by precipitation and dilution by prevailing southwesterly winds. In addition, this study used both of salinity and temperature to improve estimation of Henrys law constants (H) of PAHs in a tropical coastal area and show that correction for salinity produced 13-15% of differences in H values.

Seasonality of diffusive exchange of polychlorinated biphenyls and hexachlorobenzene across the air-sea interface of Kaohsiung Harbor, Taiwan.

Gaseous and dissolved concentrations of polychlorinated biphenyls (PCBs) and hexachlorobenzene (HCB) were measured in the ambient air and water of Kaohsiung Harbor lagoon, Taiwan, from December 2003 to January 2005. During the rainy season (April to September), gaseous PCB and HCB concentrations were low due to both scavenging by precipitation and dilution by prevailing southwesterly winds blown from the atmosphere of the South China Sea. In contrast, trace precipitation and prevailing northeasterly winds during the dry season (October to March) resulted in higher gaseous PCB and HCB concentrations. Instantaneous air-water exchange fluxes of PCB homologues and HCB were calculated from 22 pairs of air and water samples from Kaohsiung Harbor lagoon. All net fluxes of PCB homologues and HCB in this study are from water to air (net volatilization). The highest net volatile flux observed was +172 ng m(-)(2) day(-1) (dichlorobiphenyls) in December, 2003 due to the high wind speed and high dissolved concentration. The PCB homologues and HCB fluxes were significantly governed by dissolved concentrations in Kaohsiung Harbor lagoon. For low molecular weight PCBs (LMW PCBs), their fluxes were also significantly correlated with wind speed. The net PCB and HCB fluxes suggest that the annual sums of 69 PCBs and HCB measured in this study were mainly volatile (57.4 x 10(3) and 28.3 x 10(3) ng m(-2) yr(-1), respectively) and estimated yearly, 1.5 kg and 0.76 kg of PCBs and HCB were emitted from the harbor lagoon surface waters to the ambient atmosphere. The average tPCB flux in this study was about one-tenth of tPCB fluxes seen in New York Harbor and in the Delaware River, which are reported to be greatly impacted by PCBs.

Distribution and source differentiation of PAHs and PCBs among size and density fractions in contaminated harbor sediment particles and their implications in toxicological assessment.

Sediment samples collected from Kaohsiung Harbor (Taiwan) were analyzed for 15 priority polycyclic aromatic hydrocarbons (PAHs) and 118 individual polychlorinated biphenyl (PCB) congeners in various particle size fractions and two density fractions. The PAHs in the low density fraction were a much more sensitive and effective indicator of the PAH source than those in the sediment as a whole. Hierarchical cluster analysis of PAH analytes in the low density sediments revealed significant differences in compositional patterns between locations and among size fractions. In the sediment samples from both study sites, the low density fraction particles had up to 155 and 150 times higher concentrations of PAHs and PCBs, respectively, than those in the corresponding high density fractions. In addition, the total toxic benzo[a]pyrene and 2,3,7,8-tetrachlorodibenzodioxin (TCDD, dioxin) equivalents in the sediment low density fractions were much higher (up to 170 and 273 times, respectively) than the corresponding high density fractions.