Elsevier

Water Research

Volume 38, Issue 16, September 2004, Pages 3558-3568
Water Research

Distributions of polycyclic aromatic hydrocarbons in surface waters, sediments and soils of Hangzhou City, China

https://doi.org/10.1016/j.watres.2004.05.013Get rights and content

Abstract

Ten polycyclic aromatic hydrocarbons (PAHs) were simultaneously measured in 17 surface water samples and 11 sediments of four water bodies, and 3 soils near the water-body bank in Hangzhou, China in December 2002. It was observed that the sum of PAHs concentrations ranged from 0.989 to 9.663 μg/L in surface waters, from 132.7 to 7343 ng/g dry weight in sediments, and from 59.71 to 615.8 ng/g dry weight in soils. The composition pattern of PAHs by ring size in water, sediment and soil were surveyed. Three-ring PAHs were dominated in surface waters and soils, meanwhile sediments were mostly dominated by four-ring PAHs. Furthermore, PAHs apparent distribution coefficients (Kd) and solid foc-normalized Kd (e.g. Koc= Kd / foc) were calculated. The relationship between log Koc and log Kow of PAHs for field data on sediments and predicted values were compared. The sources of PAHs in different water bodies were evaluated by comparison of Koc values in sediments of the river downstream with that in soils. Hangzhou section of the Great Canal was heavily polluted by PAHs released from industrial wastewater in the past and now PAHs in sediment may serve as sources of PAHs in surface water. PAHs in Qiantang River were contributed from soil runoff. Municipal road runoff was mostly contributed to West Lake PAHs.

Introduction

Polycyclic aromatic hydrocarbons (PAHs) are a class of diverse organic compounds containing two or more fused aromatic rings of carbon and hydrogen atoms. They are ubiquitous pollutants formed from the combustion of fossil fuels and are always found as a mixture of individual compounds. Because many PAHs and their derivatives are strongly potent carcinogens and/or mutagens, the source, occurrence, transport and fate of PAHs in natural environments have been extensively studied (Liu et al., 2001; Manoli and Samara, 1999; Means et al., 1980; Chiou et al., 1998; Karickhoff et al., 1979; WHO (1998), WHO (1998)).

PAHs as one of the typical persistent organic compounds (POPs) featured in regional and global cycling (Jones and Voogt, 1999). PAHs are emitted mainly into the atmosphere and have been detected at long distances from their source (McVeety and Hites, 1988). Because of their low vapor pressures, compounds with five or more aromatic rings exist mainly adsorbed to airborne particulate matter, such as fly ash and soot. Those with four or fewer rings will occur both in the vapor phase and adsorbed to particles (Jones and Voogt, 1999; McVeety and Hites, 1998; Baker and Eisenreich, 1990). PAHs reach the hydrosphere and pedosphere mainly by dry and wet deposition and road runoff but additionally from industrial wastes containing PAHs and leaching from creosote-impregnated wood. PAHs are adsorbed strongly to the organic fraction of sediments and soils. Therefore, it can be concluded that sediments and soils are usually considered as the main sinks for PAHs in the environment and PAHs with four or more aromatic rings are persistent in the environment(Mackay et al., 1992).

In order to minimize or prevent adverse effects of POPs, many studies illustrate the fate of POPs (e.g., PAHs) in natural environments. In the past 20 years, numerous important researches focused on transport of POPs in multimedia environment (Chiou et al., 1998; Karickhoff et al., 1979), e.g., between vapor phase/particle phase in atmosphere, sediment/water, soil/water, biota/water and water/air. Chiou et al. (1979), Chiou et al (1998)) and Karickhoff et al. (1979) believed that POPs sorption into soil or sediment was dominated by partition into solid organic matter. POPs small changes in the mass of soils/sediments had a major impact on concentrations in ‘adjacent’ media, such as air or water. The partition coefficients of POPs with soils and sediments (i.e., Kd) are important parameters to characterize the mobility and fate of POPs in soil/sediment–water systems.

The measured partition coefficients of naphthalene, phenanthrene, and pyrene between soil/sediment organic matter and water (i.e., Koc) are relatively invariant either for the “clean” (uncontaminated) soils or for the clean sediments; however, the mean Koc values on the sediments are about twice the values on the soils (Chiou et al., 1998). The mean Koc values of carbon tetrachloride and 1,2-dichlorobenzene on normal bed sediments are also about twice those on normal soils (Chiou, 1998). The results indicate that conversion of eroded soils into bed sediments bring about a change in the organic matter property. The difference between soil and sediment Koc values provides a basis for identifying the source of suspended solids in river waters (Chiou, 1998; Chiou et al., 1998). The Koc values on contaminated soils and sediments are 5–10 times that of uncontaminated soils and sediments (Chiou, 1998). It was similar by reported by Sun and Boyd (1990) that non-polar solutes exhibit unusually high Koc values in soils contaminated by petroleum and/or polychlorinated biphenyl (PCB) oils. The very high Koc values observed for some special soils and sediments are diagnostic of severe anthropogenic contamination(Chiou, 1998).

PAHs occurrence in some European river waters (Manoli and Samara, 1999; Sorrell et al., 1980; Koelmans et al., 1997), seawater and sediments (Manoli and Samara, 1999; Kilikidis et al., 1994; Witt, 1995; Gustafson and Dickhut, 1997; Law et al., 1997) were extensively investigated. In China, the major investigation focused on PAHs concentrations of offshore water and sediments (Zhou and Maskaovi, 2003; Mai et al., 2001). Liu et al. (2001) and Wang et al. (2002) extensively surveyed the concentration and sources’ contribution of particulate and vapor PAHs in indoor and outdoor air of Hangzhou, China. However, until now there is little information about PAHs pollution in surface water, sediments and soils of city in China. The original objectives of this study were to survey PAHs pollution in surface water, sediments and soils in four water bodies. Another purpose was to calculate distribution coefficients (Kd) and organic carbon normalized distribution coefficients (Koc*) of PAHs in different water bodies and then evaluate PAHs contaminated sources, at the levels of water body of Hangzhou.

Section snippets

Sampling

Hangzhou is located between 30o16′ north latitude and 120o12′ east longitude, on the southeastern coastline of China, and is located in the Yangtze River Delta of China, about 150 km southwest of Shanghai. Hangzhou is the capital city of Zhejiang Province, and the population of the city is about 3.65 million, and the urban area is about 3068 km2. Located at the joint of the middle and north semitropical area, Hangzhou has a warm and humid climate with four distinct seasons, sufficient sunshine

PAHs in surface waters

The concentrations of individual and the total of 10 PAHs in water samples of four water bodies are shown in Table 3. The total concentrations of 10 PAHs in water ranged from 0.989 μg/L at Shaoniangong to 9.663 μg/L at Zhakou, with a mean concentration of 3.717 μg/L. The composition pattern of PAHs in water by ring size is shown in Fig. 2. It is clear that three-ring PAHs (fluorence, phenanthrene, and anthracene) are the most abundant in all water samples. Four-Ring PAHs (fluoranthrene, pyrene,

Acknowledgements

This study was supported by the Project of National Basic Research Program of China (2003 CB415004), the Project of National Natural Science Foundation of China (No. 20337010, 20207007), the Project of the Science and Technology Department of Zhejiang Province (001103156) and the Project of the Natural Science Foundation of Zhejiang Province (No. Z203111).

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