Biological risk and pollution history of polycyclic aromatic hydrocarbons (PAHs) in Nansha mangrove,South China

Chinese government has taken various measures to alleviate pollution caused by polycyclic aromatic hydrocarbons (PAHs) in the region of Pearl River Delta since the economic reform in 1978, but the effectiveness of these measures remains largely unknown. This study aimed to elucidate the biological risk and pollution history of PAHs by measuring the concentrations of 28 PAHs in the surface and core sediments, respectively, in Nansha mangrove. Results found that the biological risk of PAHs was low without obvious spatial variation. The PAH concentration along the depth gradient indicated that PAH pollution was stabilized since the early 1990s while the source of PAHs has gradually changed from combustion of coal to petroleum products. This implied that the mitigation measures taken by the Chinese government were effective. Compared to marine bottom sediment, we propose that using mangrove sediment can provide a more accurate and precise estimate of pollution history of PAHs.     

Temporal variation of suspended sediment load in the Pearl River due to human activities

Data on sediment flux at three hydrologic stations from the 1950s to 2006 are utilized to study the decadal,annual,and monthly variations in suspended sediment load delivered from the Pearl River to the ocean.Results show that variations in sediment flux from three main tributaries,including the West River,the North River and the East River,are spatially non-uniform.Since nearly 90%of the suspended sediment load comes from the West River,its variation has dominated the overall tendency of sediment flux in the entire Pearl River.Although a significant decreasing trend exists in the annual variation of the total sediment flux,the decadal change can be divided into an increasing phase and a decreasing phase,with the turning point between the two phases in the late 1980s.From the 1950s to the 1980s,the average annual river sediment flux increased by 30.43%.However,sediment flux has decreased significantly since the 1990s,with the average sediment flux being 38.60%less in the 2000s than that in the 1950s.The current sediment flux is also 52.93%less than its peak in the 1980s. The monthly variation pattern of the suspended sediment load transport to the sea is more interesting. For the West River,all months show a decreasing trend,and for most months the reduction values are significant.However,for the East River the sediment load shows a decrease trend in the dry season and an increase trend in the wet season.The method of regression analysis was used to study the influence of precipitation in the variation on the sediment flux.It was found that the climate change is not the main driving force behind the variation in suspended sediment load.Before the 1990s, intensive land use destroyed the vulnerable ecosystem of the upper Pearl River,and speeded up the process of rocky desertification.Consequently,aggravated soil erosion caused an increase in suspended sediment load.However,sediment retention within reservoirs had begun to play a dominant role after the massive construction of large dams after 1990,and resulted in a decrease in the suspended sediment load delivered to the ocean.     

Risks posed by trace organic contaminants in coastal sediments in the Pearl River Delta, China

Local marine environments in China's Pearl River Delta (PRD), the most rapidly developing region in one of the world's fastest growing economies, have been experiencing significant environmental stress during the past decades. This investigation was conducted to determine the status and trends of persistence organic pollutants (POPs) such as polycyclic aromatic hydrocarbons (PAHs), petroleum hydrocarbons (PHCs), polychlorinated biphenyls (PCBs), organochlorine (OC) pesticides and dioxin-related compounds in marine sediments collected from sixteen coastal stations in the Pearl River Delta (PRD) in March 2003. Elevated concentrations of PAHs (94-4300 ng/g), PCBs (6.0-290 ng/g), PHCs (14-150 microg/g), and DDTs (1.4-600 ng/g) were detected in sediment samples. In addition, 2,3,7,8-tetrachlorodibenzo-p-dioxin (TCDD)-like activities in the sediment samples were estimated to range from 0.3 to 440 pg TCDD-EQ/g. Sediments collected from Xiashan contained the greatest concentrations of trace organic contaminations amongst all the sampling stations in the present study. The degree of trace organic contamination was, in general, more severe at stations situated along the west shores of the PRD than their counterparts in the east. A preliminary assessment was performed to examine the probable risks to the marine ecosystem due to POPs. The results showed that OC pesticide contamination in the PRD was particularly serious and might pose a threat to the health of the marine inhabitants.     

In-situ partitioning and bioconcentration of polycyclic aromatic hydrocarbons among water,suspended particulate matter,and fish in the Dongjiang and Pearl Rivers and the Pearl River Estuary,China

The partitioning and bioaccumulation of polycyclic aromatic hydrocarbons (PAHs) in water, suspended particulate matter (SPM), and fish samples from the Dongjiang River (DR), Pearl River (PR), and the Pearl River Estuary (PRE) were examined. Although PAHs are much lower in PRE than in DR or PR, PAHs in some fish species are significantly higher in PRE than in DR or PR. Aqueous or particulate PAHs respectively show significant correlations with dissolved organic carbon, particulate organic matter, and chlorophyll a, suggesting that biological pumping effect regulates their distribution. The in situ partitioning coefficients (log K_oc) for PAHs are one order magnitude higher than the empirical log K_oc–log K_ow correlation. The bioconcentration factor (BCF) is slightly higher for the marine fish than for the freshwater fish. The above phenomena indicate that BCF may vary due to the diversity of fish species, feeding habits, and metabolism of PAHs in fish.     

TEMPORAL AND SPATIAL DISTRIBUTIONS OF PAHS AND PCBS IN LAKE CALUMET AREA, CHICAGO

1 INTRODUCTION Lake Calumet is located 15 miles southeast of downtown Chicago. The geographical boundaries include 130th Street to the south, Stony Island Avenue to the east, an industrial area to the north, and interstate highway I-94 to the west. The major continuous water inflow to the lake is Pullman Creek, a drainage ditch, which carries the runoff from the nearby expressway, industries, and landfills into the lake at the northwest corner. The outlet of the Lake is the Calumet R…     

Assessment of polycyclic aromatic hydrocarbon input to urban wetlands in relation to adjacent land use

The relationship between polycyclic aromatic hydrocarbons (PAHs) in wetland surface sediments and adjacent land use was assessed in the Elizabeth River, VA, an urbanized sub-estuary of the Chesapeake Bay. Significant differences (p<0.05) in surface sediment PAH concentration between sites indicated adjacent land use had a substantial influence on PAH concentration in wetland sediments. Wetlands adjacent to parking lots and petroleum industrial sites exhibited the highest PAH concentrations of all wetlands examined. Overall, commercial land uses had the highest PAH concentrations and automotive sources dominated (52-69%) PAH input to wetland surface sediments irrespective of adjacent land use.     

Distribution and origins of polycyclic aromatic hydrocarbons (PAHs) in riverine, estuarine, and marine sediments in Thailand

To assess the status of polycyclic aromatic hydrocarbon (PAH) contamination in coastal and riverine environments in Thailand, we collected 42 surface sediment samples from canals, a river, an estuary, and coastal areas in Thailand in 2003 and analyzed them for PAHs with 3-7 benzene rings by gas chromatography-mass spectrometry (GC-MS). The total concentration of PAHs ranged from 6 to 8399 ng/g dry weight. The average total PAH concentrations were 2290+/-2556 ng/g dry weight (n=8) in canals, 263+/-174 (n=11) in the river, 179+/-222 (n=9) in the estuary, and 50+/-56 (n=14) in coastal areas. Comparison of the concentration range with a worldwide survey of sedimentary PAH concentrations ranked PAH contamination in Thai sediments as low to moderate. The ratio of the sum of methylphenanthrenes to phenanthrene (MP/P ratio) allows discrimination of PAH sources between petrogenic (>2) and pyrogenic (<0.5) origins. Sediments from urban canals in Bangkok showed the highest PAH concentrations and petrogenic signatures (MP/P=1.84+/-0.98 [n=6] in canal sediments) with abundant alkylated PAHs, indicating major sources of petrogenic PAHs in the city. To identify the sources of the petrogenic inputs in Thailand, we analyzed triterpanes, biomarkers of petroleum pollution, in the sediment samples and in potential source materials. Hopane profiles were remarkably uniform throughout the nation, suggesting a diffuse single source (e.g. automobiles). Molecular profiles of hopanes and PAHs in sediments from the urban canals were similar to those in street dust, indicating that street dust is one of the major sources of petrogenic PAHs in the urban area. On the other hand, low levels of PAHs (approximately 50 ng/g) with a pyrogenic signature (MP/P ratio approximately 0.5) were widely recorded in remote areas of the coast and the Chao Phraya River. These pyrogenic PAHs may be atmospherically transported throughout the nation. Middle and lower reaches of the Chao Phraya River, the river mouth, and the upper Gulf of Thailand showed intermediate concentrations and profiles of PAHs, indicating mixtures of petrogenic and pyrogenic origins. Perylene was abundant in sediments, representing up to approximately 60% of total identified PAHs. High inputs of soil due to frequent heavy rains could contribute to the high perylene abundance in the sediments. Sedimentary PAH concentrations decreased offshore with a half distance of approximately 10 km in the upper Gulf off the mouth of the Chao Phraya River. This is probably due to active deposition of laterally transported riverborne particles.     

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.     

Occurrence and phase distribution of polycyclic aromatic hydrocarbons in riverine runoff of the Pearl River Delta, China

The occurrence and phase distribution of polycyclic aromatic hydrocarbons (PAHs) in waters at the eight riverine outlets of the Pearl River Delta (China) were examined based on a monthly sampling program from March 2005 to February 2006. The total concentrations of PAHs in the aqueous phase and suspended particulate matter (SPM) combined ranged from 55.5 to 522 ng/L, at the mid level of the global values in rivers and estuaries. No clear temporal and spatial trends of PAH concentrations were found. However, the concentrations of PAHs associated with SPM coincided with the monthly precipitation of Guangzhou, indicating the importance of atmospheric deposition. The PAHs found in the region were likely derived from a combined pyrolytic and petrogenic origin, as suggested by the molecular indices of PAHs. Normalized partition coefficient (K(oc)) between water and SPM was correlated with octanol-water partition coefficient (K(ow)) to understand the environmental behavior of PAHs.     

Reconstruction of pollution history of organic contaminants in the upper Gulf of Thailand by using sediment cores: first report from Tropical Asia Core (TACO) project

This paper reports the first reconstruction of a pollution history in tropical Asia from sediment cores. Four sediment core samples were collected from an offshore transect in the upper Gulf of Thailand and were analyzed for organic micropollutants. The cores were dated by measurement of (137)Cs and geochronometric molecular markers (linear alkylbenzenes, LABs; and tetrapropylene-type alkylbenzenes, TABs). Polychlorinated biphenyl (PCB) concentrations showed a subsurface maximum in layers corresponding to the 1970s, indicating the effectiveness of regulation of PCBs in Thailand. LAB concentrations increased over time, indicating the increase in input of sewage into the Gulf during the last 30 years. Hopanes, biomarkers of petroleum pollution, also increased over time, indicating that the inputs of automobile-derived hydrocarbons to the coastal zone has been increasing owing to the increased number of cars in Thailand since the 1950s. Polycyclic aromatic hydrocarbons (PAHs) increased in the layers corresponding to the 1950s and 1960s, probably because of the increased inputs of automobile-derived PAHs. PAH concentrations in the upper layers corresponding to the 1970s and later remained constant or increased. The absence of a subsurface maximum of PAHs contrasts with results observed in industrialized countries. This can be explained by the facts that the Thai economy did not depend on coal as an energy source in the 1960s and that economic growth has continued since the 1970s to the present. The deposition flux of PAHs and hopanes showed a dramatic offshore decrease, whereas that of LABs was uniform.     

Spatio-temporal distribution and characteristics of PAHs in sediments from Masan Bay, Korea

The distribution of polycyclic aromatic hydrocarbons (PAHs) has been investigated in the surface and core sediments from Masan Bay, Korea. Total PAHs in the surface sediments ranged from 207 to 2670 ng/g dry weight with a mean value of 680 ng/g. Qualitative similarity and quantitative difference between inner and outer bay indicate that the main sources of PAHs are located in the inner bay and outer bay is also affected by the same sources. Vertical distribution of PAHs revealed that three distinctive stages could be differentiated with the help of PCA analysis. The highest concentration (industrialization stage) appeared between late 1950s and 1980, which was 10 years later than other developed countries. A strong pyrolytic source fingerprint has been detected with slight influence of petrogenic sources, and diagenetic PAH, perylene also contributed. Total organic carbon normalized PAHs (sum of 13 PAHs, 8.85-88.0 microg/g OC) were under the threshold effects concentration (TEC, 290 microg/g OC).     

PAH-profiles in sediment cores from the Baltic Sea

To document the historical input the PAH-profiles of sediment cores in two different basins of the Baltic Sea, the Gotland Basin (GB) and Arkona Basin (AB), were analysed by means of GC-MS. 35 PAHs were quantified in all samples, and additionally, several marker PAHs, like Cyclopenta[cd]phenanthrene (CCP) for combustion processes and retene for terrigenous input, were quantified in selected samples. The preindustrial sediments (older than 200-250 years) in the GB core illustrate concentrations <100 ng PAH15 g(-1) d.w. Calculated PAH-ratios indicated combustion processes as the main sources for both basins. The Perylene concentrations within the sediment cores decrease with increasing depth, along with an increase in relative percentage, indicating slow diagenetic processes. The preservation and enrichment of the introduced PAHs was more pronounced in the GB core.     

The formation mechanisms of turbidity maximum in the Pearl River estuary, China

The formation and dynamics of turbidity maxima (TM) in the Pearl River estuary (PRE) are not well understood but the existence of TM in the estuary have great potential engineering and environmental impacts. Based on the measurements of two large-scale field surveys conducted in the wet season of 1978 (July of 1978) and the dry season of 1979 (March of 1979), the existence and seasonal variations of TM in the PRE focusing on the two major natural navigation channels have been studied. The sediment transport fluxes over two consecutive tidal cycles have been analyzed in detail. The analysis results reveal that the formation mechanisms of TM in the estuary are rather complex. In general, gravitational circulation, tidal trapping, and sediment resuspension and deposition processes are the primary TM formation mechanisms in the PRE. The clockwise back flow pattern around Lingding Island also leads to the formation of TM in the West channel of the PRE. The occurrence of TM far upstream of the salt water wedge is the result of the complex hydrodynamic and sediment transport processes generated by the runoff of the major rivers.     

Distribution and characteristics of PAHs in sediments from the Mediterranean coastal environment of Egypt

To assess the contamination of polycyclic aromatic hydrocarbons (PAHs) in the Mediterranean coastal environment of Egypt, 26 sediment samples from the coastline, harbours, estuaries and coastal lakes were collected and analyzed. The sediment PAH concentrations of thirty-nine 2-6 ring PAHs ranged from 13.5 to 22,600 ng/g. PAH profiles varied according to the nature of the site and its proximity to sources. Industrialized and urbanized region showed high level of PAHs contamination. In general, the contamination levels of PAHs were similar to those observed in contaminated and slightly contaminated sediments of the Mediterranean Sea. Molecular indices based on ratios of selected PAH concentrations were used to differentiate PAHs from pyrogenic and petrogenic and mixed origins. Good correlations were observed between the petrogenic index, MP/P, A-PAHs/P-PAHs and HMW/LMW. Finally, PAH levels in sediments were compared with Sediments Quality Guidelines (ERM-ERL) for evaluation of probable toxic effects on organism.     

Occurrence and phase distribution of polycyclic aromatic hydrocarbons in riverine runoff of the Pearl River Delta,China

The occurrence and phase distribution of polycyclic aromatic hydrocarbons (PAHs) in waters at the eight riverine outlets of the Pearl River Delta (China) were examined based on a monthly sampling program from March 2005 to February 2006. The total concentrations of PAHs in the aqueous phase and suspended particulate matter (SPM) combined ranged from 55.5 to 522 ng/L, at the mid level of the global values in rivers and estuaries. No clear temporal and spatial trends of PAH concentrations were found. However, the concentrations of PAHs associated with SPM coincided with the monthly precipitation of Guangzhou, indicating the importance of atmospheric deposition. The PAHs found in the region were likely derived from a combined pyrolytic and petrogenic origin, as suggested by the molecular indices of PAHs. Normalized partition coefficient (K_oc) between water and SPM was correlated with octanol–water partition coefficient (K_ow) to understand the environmental behavior of PAHs.     

Dynamic behaviour of polycyclic aromatic hydrocarbons in Brighton marina, UK

The distribution of polycyclic aromatic hydrocarbons (PAHs) between various phases is fundamental in the control of their movement and impact in the marine environment. In this study samples of water and sediments were regularly collected from Brighton marina, UK, to quantify the intensity, spatial and temporal variations of PAH contamination. The results show clearly that PAH behaviour in marine systems is highly complex, and controlled by the interplay of PAH sources, compound physicochemical properties, water and sediment movement, and field conditions. Levels of total PAHs (16 compounds) in the dissolved phase were found to vary between <2 and 11,400 ng/l, with higher values observed in the winter months. Total PAH concentration in sediment samples varied between 24 and 4710 ng/g dry weight. PAHs in water were dominated by low molecular mass compounds (2-ring), while PAHs in sediments were mainly derived from 2-4 ring compounds. In addition, dissolved concentrations were increased during sediment dredging and after a period of severe rainfall. PAHs in Brighton marina are likely to be from both pyrolytic and petrogenic sources; as a result, field-derived distribution coefficients for individual PAHs between sediment and water tend to follow the equilibrium partition models, although slight exceedance is apparent. The extended partition model incorporating soot carbon has achieved limited success in better predicting PAH behaviour.     

Riverine inputs of total organic carbon and suspended particulate matter from the Pearl River Delta to the coastal ocean off South China

A total of 1008 samples were collected from the eight major riverine runoff outlets in the Pearl River Delta (PRD) during 2005-2006 to estimate the fluxes of total organic carbon (TOC) to the coastal ocean off South China. The average dissolved organic carbon (DOC) concentration was 1.67 mg/L with a range of 1.38-2.13 mg/L. Concentrations of particulate organic carbon (POC) ranged from 2.66-4.12% of total suspended particulate matter (SPM). The fluxes of TOC and SPM from the PRD via the eight outlets were 9.2 x 10(5) and 2.5 x 10(7)tons/yr, respectively. Temporal variations in POC and DOC were observed at all outlets due to the large variability in runoff levels because of the seasonality of rainfall, and the riverine discharge amount was an important factor controlling TOC flux. The net contribution of organic carbon from the PRD to the coastal ocean represented approximately 0.1-0.2% of total organic carbon transported by rivers worldwide.     

Inhomogeneous distribution of polycyclic aromatic hydrocarbons in different size and density fractions of contaminated sediment from Auckland Harbour, New Zealand: an opportunity for mitigation

Polycyclic aromatic hydrocarbons (PAHs) in sediment from Auckland Harbour (New Zealand) are not distributed evenly throughout bulk sediment, but highly concentrated in coarser, low-density fractions. Concentrations of 24 PAHs, measured in sediment that was separated into six size fractions that were furthermore separated into two density sub-fractions by flotation in sodium-polytungstate solution (rho = 2.15 g cm(-3)), varied between 4-103 microg g(-1)dw among grain size fractions and 2-998 microg g(-1)dw for density sub-fractions. Highest PAH concentrations were measured in the low density, 125-250 microm fraction. All sediment fractions had a similar relative PAH composition, dominated by >3-ring PAHs, suggesting a common pyrogenic origin. Low density material had 10-200 times higher PAH concentrations and 10-100 times higher organic carbon (OC) content, yet differences in OC content only partially accounted for variations in PAH concentration. Low density particles contributed more than 75% of the Sigma PAH, while comprising only 3% of bulk sediment dry weight. This may have significant utility for contaminant mitigation efforts in Auckland Harbour.     

Comprehensive assessment of heavy metal contamination in sediment of the Pearl River Estuary and adjacent shelf

Total metal concentrations (Cr, Ni, Cu, Zn, and Pb), acid volatile sulfide and simultaneously extracted metals (AVS-SEM), and heavy metal fractionation were used to assess the heavy metals contamination status and ecological risk in the sediments of the Pearl River Estuary (PRE) and adjacent shelf. Elevated concentrations at estuarine sites and lower concentrations at adjacent shelf sites are observed, especially for Cu and Zn. Within the PRE, the concentration of heavy metals in the western shore was mostly higher than that in the middle shore. The metals from anthropogenic sources mainly occur in the labile fraction and may be taken up by organisms as the environmental parameters change. A combination of total metal concentrations, metal contamination index and sequential extraction analysis is necessary to get the comprehensive information on the baseline, anthropogenic discharge and bioavailability of heavy metals.     

Survey of PAH in low density residential stormwater ponds in coastal South Carolina: false dark mussels (Mytilopsis leucophaeata) as potential biomonitors

The distribution of PAHs was studied in sediment and false dark mussels, Mytilopsis leucophaeata, of three brackish stormwater retention ponds on Kiawah Island, a gated residential community and golf resort. Impervious surface in pond watersheds ranged from 5 to 30%. Sediment concentrations were lower than those found in other studies of suburban residential areas, and there were no significant differences among ponds or seasons. Mean summation operatorPAH(16) values for sediments in Ponds 67, 100, and 37 were 184.7+/-101.3ng g(-1), 67.5+/-26.0ng g(-1), and 84.3+/-75.5ng g(-1), respectively. Mussel summation operatorPAH(16) concentrations from Pond 67 in August (mean 734.5+/-148.1ng g(-1)), and from Pond 37 in December (mean 1115.1+/-87.7ng g(-1)), were significantly higher than other ponds. Mean summation operatorPAH(16) values for mussels in Ponds 67, 100, and, 37 were 555.9+/-219.7ng g(-1), 312.5+/-99.1ng g(-1) and 737.8+/-419.8ng g(-1), respectively. The mean biota-to-sediment ratio was 7.6+/-8.1. Isomer ratios generally suggested pyrogenic sources. False dark mussels are a promising indicator species for PAH contamination because they are abundant, easy to sample, bioaccumulate PAH profiles representative of the time-integrated sediment profiles, and their PAH levels are less variable than either stormwater or sediment samples.